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cellulose fibers composite for photocatalytic application
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In-situ synthesis of BiVO4 QDs/cellulose fibers composite for photocatalytic application Tao Wang a,d, Xiqing Liu b, Donglai Han d, Yuxuan Sun e, Changchang Ma c,d,**, Yang Liu d,f, Pengwei Huo c,d, Yongsheng Yan c,d,* a
School of the Environmental and Safety Engineering, Jiangsu University, 212013, Zhenjiang, PR China School of Material Science and Engineering, Jiangsu University, 212013, Zhenjiang, PR China c School of Chemistry and Chemical Engineering, Jiangsu University, 212013, Zhenjiang, PR China d Institute of Green Chemistry and Chemical Technology, Jiangsu University, 212013, Zhenjiang, PR China e College of Chemistry, Jilin Normal University, 13600, Siping, PR China f College of Physics, Jilin Normal University, 13600, Siping, PR China b
highlights
graphical abstract
Bamboo as the source to prepared cellulose fibers due to its abundant and short growth cycle. A novel BiVO4 QDs/fibers composite photocatalyst was obtained via the in-situ method. Rich groups of natural cellulose fibers provided many sites to form the
stability
and
distribution
BiVO4. The mechanism of synthesis and the photocatalytic process were discussed and proposed.
article info
abstract
Article history:
In this work, a biofiber was used as the natural polymer carrier to design a BiVO4 QDs/
Received 25 July 2019
cellulose fiber composite for photocatalytic application. The biofiber was obtained from
Received in revised form
bamboo, which was green, abundant and short growth cycle in Asia. Naturally rich
16 September 2019
groups of biofiber provided many sites to absorb the Bi3þ to form the uniform distribution
Accepted 12 October 2019
for BiVO4 QDs. Moreover, a series of results indicated the strong connection was formed
Available online xxx
between biofiber and BiVO4 QDs, which could increase the stability and electron transfer. Therefore, the new composite photocatalyst exhibited better stability and effectively
Keywords:
photocatalytic
activity.
Moreover,
the
possible
mechanism
of
synthesis
and
Biomaterials
* Corresponding author. School of Chemistry and Chemical Engineering, Jiangsu University, 212013, Zhenjiang, PR China. ** Corresponding author. E-mail addresses: [email protected] (C. Ma), [email protected] (Y. Yan). https://doi.org/10.1016/j.ijhydene.2019.10.096 0360-3199/© 2019 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved. Please cite this article as: Wang T et al., In-situ synthesis of BiVO4 QDs/cellulose fibers composite for photocatalytic application, International Journal of Hydrogen Energy, https://doi.org/10.1016/j.ijhydene.2019.10.096
2
international journal of hydrogen energy xxx (xxxx) xxx
Natural cellulose fiber
photocatalytic were discussed, which provided insight for synthesizing photocatalytic
Chemical bonding
based on biomaterials.
Photocatalytic
© 2019 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.
BiVO4 QDs
Introduction Since the development of industrial, the growing pollution and destruction have caused serious problem [1e4]. Fortunately, new photocatalytic technology has been developed and it could apply in water splitting, CO2 conversion and organic removal via convert nature solar energy, thus attracting much attention [5e7]. Bismuth vanadium oxide (BiVO4, BVO) was one of newly photocatalytic material and possessed narrow bandgap, outstanding chemical stability, thus it has been known as a feasible visible-light-driven material [8e10]. Nevertheless, the common BVO has been limited by light response efficiency. Many researchers demonstrated that quantum-sized materials have widely investigated and applied in photoelectric devices, photocatalysis, and others due to their unique properties [11,12]. Therefore, many quantum sized semiconductor materials were developed and used in the photocatalytic fields, such as CdS, ZnO, ZnSe and so on [13e15]. As expected, quantum-sized BVO has prepared and Sun et al. making it be a photocatalyst for H2 evolution due to quantum confinement effect [16]. Unfortunately, quantum-sized materials are easily to aggregate because of high surface energy, resulted in poor stability and low catalytic activity. Generally speaking, constructing composite photocatalyst could increase the stability of quantum sized materials [17]. Meanwhile, composite photocatalyst would exhibit better catalytic activity than pristine material [18,19]. For example, Wang's group reported that vanadate quantum dots (QDs) interspersed g-C3N4 could enhance efficient inactivation of Salmonella via absorbing light source [20]. Li et al. reported a BVO QDs decorated BiPO4 nanorods via in-situ growth method, which also increased visible-light-driven photocatalytic activity [21]. Luo et al. designed a CuInS2 QDs/BiWO6 photocatalyst, resulting in higher photocatalytic activity due to the configuration of p-n heterojunction and simultaneously tune the behavior of photogenerated charge carriers [22]. An ideal substrate for BVO QDs, efficient and environmentally friendly, should be developed. Cellulose, one of the most abundant biopolymer on Earth, which has appealing mechanical properties, special modulus and special strength [23,24]. Among, bamboo fiber was the main natural source of cellulose and widely distributed in Asia. Bamboo, an ideal source of cellulose fiber (CF) due to their preponderance of the breeding fast, good renewability, high yield, wide-ranging and environmentally friendly [25e27]. Cellulose, the structure of the superfine network not only provides mechanical support but also benefit to disperse the nanoparticles and enhance the photocatalyst stability. In addition, the hydroxyl groups in the cellulose structure could
connect with semiconductor oxide particles. Some reports have demonstrated that the semiconductor oxide particles into a cellulose polymer matrix showed enhanced properties. For example, Mohamed M.A. et al. incorporated NeTiO2 nanorods in cellulose membrane matrix, forming a strong interaction between the hydroxyl groups of cellulose and TiO2 through bonding interactions [28]. In this work, the novel BVO QDs/nature cellulose fiber composite were obtained through in situ growth method under ultrasound with use of bamboo as the cellulose source. The formation process of BVO QDs decorated on cellulose fiber and the possible bonding effect was discussed. The physicochemical characteristic of BVO-cellulose fiber composite was studied. Moreover, the photocatalytic performance of BVOcellulose fiber composite was determined by the degradation of the organic pollutant aqueous solution. As a result, the stability of BVO QDs was enhanced via the interaction with hydroxyl groups of cellulose, and the charge carrier transfer on the BVO-cellulose fiber resulted in improved the photocatalytic activity. The crystal structure, photocatalytic mechanism, chemical groups of the BVO-cellulose fiber composite were studied for open up a simple, effective and economic strategy toward the design of unique nature cellulose-based materials, which may provide a practical visible-light photocatalyst.
Experimental Chemicals Bamboo from Jiangsu University campus. Bismuth nitrate pentahydrate (Bi(NO3)3‧5H2O), ammonium metavanadate (NH4VO3), sodium sulfite (Na2SO3) tetracycline (TC) and citric acid monohydrate (C6H8O7‧H2O, CA) were obtained from Aladdin chemistry Co. Ltd (Shanghai, China). Ammonia solution (NH3H2O), ethanol (C2H5OH), isopropyl alcohol (C3H7OH, IPA), hydrogen peroxide solution (H2O2) and sodium hydroxide (NaOH) were purchased from Sinopharm Chemical Reagent Co., Ltd (Shanghai, China). All reagents were all of the analytic grades and used without a further treat. The deionized water used throughout the whole experiment.
Natural cellulose fiber obtained from bamboo As we known, bamboo stems were mainly composed of cellulose, hemicellulose, lignin and other chemicals. Thus, it was necessary to gradually remove other components except for cellulose. The bamboo cut into small species and washed for the following treatment. The mixed solution was consisted of by dissolving NaOH (2.5 M) and Na2SO3 (0.4 M) in deionized
Please cite this article as: Wang T et al., In-situ synthesis of BiVO4 QDs/cellulose fibers composite for photocatalytic application, International Journal of Hydrogen Energy, https://doi.org/10.1016/j.ijhydene.2019.10.096
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water. The bamboo species was immersed in the mixed solution and kept boiling for 24 h, followed by rinsing in deionized water to remove the chemicals. Then, the bamboo species were placed in the 2.5 M H2O2 solution for boiling without stirring. When the green bamboo changed to white, the sample was filtered and washed with deionized water. The cellulose was obtained from the above process, and drying for further experiments.
The preparation of BiVO4 quantum dots/cellulose fiber composite The composite was prepared via a simply in suit ultrasonic method. Firstly, the cellulose fiber was added into Bi(NO3)3‧ 5H2O (30 mL, 5 mM) solution under ultrasound to form a uniform suspension. Then, the NH4VO3 solution (30 mL, 5 mM) was added into the suspension solution with strongly stirring and ultrasound. Next, the pH of the solution was adjusted to 7 with NH3‧H2O solution. The obtained precipitates were centrifugation, washed with deionized water and ethanol, and dried at low temperature. The pure vanadate QDs was synthesized by the same process without added cellulose fiber. The theoretical weight ration of cellulose fiber in the BiVO4 QDs/cellulose fiber was 15 wt%, 10 wt%, 5 wt% and 1 wt%, the corresponding samples were marked as BCF-1, BCF-2, BCF-3 and BCF-4, respectively.
Photocatalytic experiment The photocatalytic performance of BCF composite was determined by the degradation and 300 W Xe lamp (cut off 420 nm) as the light source. The photocatalyst (20 mg) was dispersed in 100 mL 10 mg/L TC solution by violent stirring to achieve an adsorption-desorption equilibrium under dark conditions. Then, the suspension was exposed to light illumination with stirring. At each time interval, 4 mL of suspension was collected to remove the photocatalyst, and the absorption of TC solution was applied to analyze its degradation by UV-2700 spectrophotometer.
Material characterization The crystal structure of the samples was determined by X-ray diffraction (XRD). The morphology of samples was observed by field-emission electron microscope (FE-SEM), and the
3
elemental distribution of composite was analyzed by corresponding SEM with X-ray energy dispersive spectroscopy (EDS). Fourier transform infrared spectra (FT-IR) was used to decide the chemical groups. The surface chemical analyses of the sample were carried out by X-ray photoelectron spectroscopy (XPS). The Brunauer-Emmett-Teller (BET) surface areas of prepared samples were determined via N2 adsorption isotherms. Further structural was analyzed by Raman spectroscopy. The optical absorption spectra and diffuse reflection spectra were analyzed by UVevis spectrophotometer with an integrating sphere.
Results and discussion The formation process of BiVO4 QDs-cellulose fibers The preparation process and possible mechanism of BVO QDs loaded on cellulose fiber were proposed (Fig. 1). The support of cellulose fiber was obtained from bamboo through removing lignin and other ingredients. Due to sufficient hydroxy and carboxyl on the molecule chain of cellulose fiber, which provided many sites for adsorbing Bi3þ [29,30]. The BVO was started to crystallize when added the NH4VO3 solution. In order to inhibit the agglomeration by rapid crystallization of BiVO4, the reaction was kept strong stirring and ultrasound. Finally, the reaction was completed to achieve a quantum size BVO growth on the surface of cellulose fiber. During the reaction, the sufficient hydroxy and carboxyl not only provided the sites for the growth of BVO QDs but also could increase the stability of composite due to chemical adsorbed.
Morphology and structure analysis As Fig. 2a showed, the cellulose fiber was like a very long line, which exhibited irregular size and micron length due to the uncontrollability of biological materials [31]. These would provide enough area for the growth of BVO QDs. The SEM image of BCF composite was presented in Fig. 2b, the surface of cellulose fiber changed rough. As observed, the rough surface consisted of much nanoparticles, which may be attributed to the BVO QDs were growth in the surface of cellulose fiber [32]. In addition, the TEM images were further to observe the morphology of BCF composite. As Fig. S1a showed much nanoparticles were loaded on the surface of large fiber. The
Fig. 1 e The possible synthesis mechanism of BCF composite. Please cite this article as: Wang T et al., In-situ synthesis of BiVO4 QDs/cellulose fibers composite for photocatalytic application, International Journal of Hydrogen Energy, https://doi.org/10.1016/j.ijhydene.2019.10.096
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Fig. 2 e The SEM images of natural bamboo fibers (a) and BCF composite (b), corresponding EDS mapping (cee).
Fig. 3 e XRD patterns (a) and enlarged XRD patterns (b) of pure BiVO4 and BCF composite.
nanoparticles were ascribed to BVO QDs with the size about 10 nm, which was consistent with the SEM images. Moreover, the lattice fringe at 0.48 nm was attributed to the d-spacing of (110) of BVO (Fig. S1b), further confirming the formation of BVO QDs on fibers. Meanwhile, the corresponding EDS mapping of BCF composite further demonstrated that the BVO QDs were evenly dispersed on the apparent of cellulose fiber, which contained elements of Bi, V and O. Further verifying the BVO QDs was successfully synthesized, some characterizations were adopted. The crystal structures of prepared materials were tested via the XRD, shown in Fig. 3a. It clearly found that the diffraction peaks of BVO QDs were fully corresponding to the BVO standard card (PDF#44-0081). The intensity peaks of BVO QDs indicated that the sample has good crystallinity without impurity [33]. For the BCF composite, the diffraction peaks were still corresponding to the BVO, implying the BVO QDs
maintained the BVO crystal structure in the composite material. However, no peaks belonged to cellulose fiber, which may be attributed to the low crystallinity formed by complex organic structures. In the enlarged XRD spectra (Fig. 3b), an obviously shifted was happed in the BCF composite compared to pure BVO QDs. The changes would demonstrate the BVO QDs were growth in the cellulose fiber and were consistent with the above analysis that Bi3þ connected cellulose fiber with chemical bonding [34]. The analysis was further verified by the following examination. Raman spectroscopy was applied to study the BVO QDs’ vibrational properties and structural, the spectra were presented in Fig. 4a. For the pure BVO QDs, the intense peak at 829 cm1 was ascribed to symmetric VeO stretching mode and a weak shoulder at about 708 cm1 ascribed to asymmetric VeO stretching mode. The peaks located at about 325 and 367 cm1 were attributed to the symmetric bending mode
Please cite this article as: Wang T et al., In-situ synthesis of BiVO4 QDs/cellulose fibers composite for photocatalytic application, International Journal of Hydrogen Energy, https://doi.org/10.1016/j.ijhydene.2019.10.096
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Fig. 4 e Raman (a) and FT-IR (b) of samples.
and the asymmetric bending of vanadate anions, respectively [35,36]. Moreover, the external modes (rotation/translation) were appeared at about 127 and 211 cm1, respectively [37,38]. The result further verified the BVO QDs was prepared. For the Raman spectra of BCF composite, the peaks maintained the features of BVO QDs obviously. However, the intensity and position of peaks were changed in the BCF composite compared to pure BVO QDs, which demonstrated the BVO QDs growth in cellulose fiber with the connection of hydroxy and carboxyl. The changed of chemical groups was determined by FT-IR, which could prove the chemical interaction between BVO QDs and cellulose fiber. For pure BVO QDs, the vibration band
located at 679 cm1 could be ascribed to the asymmetric stretching vibration of the VO4 [39]. For pure cellulose fiber, the hydroxyl and carboxyl groups were detected. The peaks characterization at about 615, 1059, 1376, 1594, 2897, 2794 and 3366 cm1, were assigned to the CH2, CeOeC, C]O, CH3, CH2 and OeH, respectively [40,41]. It clearly found that primary bands of BVO QDs and cellulose fiber were included in composite, indicating the BCF composite were prepared successfully. Moreover, the peaks of chemical groups in the BCF composite were disappeared or displacement, which proved a bond connection was formed between BVO and cellulose fiber. The chemical bond would increase the stability and charge transfer of BCF composite.
Fig. 5 e XPS spectra of BVO and BCF composite, (a) survey, (b) Bi 4f, (c) V 2p and (d) O 1s. Please cite this article as: Wang T et al., In-situ synthesis of BiVO4 QDs/cellulose fibers composite for photocatalytic application, International Journal of Hydrogen Energy, https://doi.org/10.1016/j.ijhydene.2019.10.096
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Fig. 6 e N2 adsorption-desorption isotherms of BVO, cellulose fibers and BCF composite (a), Nyquist plot of BVO and BCF composite (b).
BET analysis The BET surface area of the samples was obtained by N2 adsorption-desorption isotherms [46]. As Fig. 6a showed all samples displayed a type hysteresis loop in type-III isotherm, indicating that the material did not have pores or have large pores. The results were consistent with the SEM images. According to the computer, the BET surface area of cellulose fiber, BVO QDs and BCF were 78.935, 62.561 and 29.835 m2/g, respectively. The large surface area of cellulose fiber would provide enough sites for the growth of BVO QDs. As expected, the surface area of BCF was smaller than the pure CF, indicating the BVO QDs were growth in the cellulose fiber. Generally speaking, the larger surface area would benefit to the photocatalytic activity [47]. But in this work, the BCF composite displayed better catalytic activity than pure BVO QDs, which surface area of BCF was smaller than BVO QDs, demonstrating that the electronic transfer played the main
role in the composite instead of pure materials. The better electronic transfer may be attributed to the chemical connection between cellulose fiber and BVO QDs. Thus, the electrochemical impedance spectroscopy was used to demonstrate the charge transfer abilities of the samples based on the charge transfer resistance. As general, the smaller radius size of the Nyquist plot implied the better change transfer due to the small the charge transfer resistance. From the Fig. 6b, the radius of BCF composite was smaller than pure BVO, revealing the high charge transfer rate for improving photocatalytic activity.
Optical properties The light absorption properties were an important indicator for determining whether the materials were excited by visible light [48e50], the UVevis DRS spectra were presented in Fig. 7. Obviously, the absorption edge of BCF composite was more than 500 nm, indicating the BCF composite could be excited under visible-light. However, the absorption wavelength region of BCF composite showed slight red-shift compare to pristine BVO QDs, which was attributed to the color of the cellulose fiber was white. It was worth noting that the absorbance intensity of BCF composite was increased, which was attributed to the C]C and C]O bands. Moreover, the bandgap energy of samples could be calculated through the formula [51]: 1 2
ahn ¼ Aðhn Eg Þ
=
The surface chemical state and chemical link of the BCF composite, the pure BVO and BCF composite were studied via XPS measurement. As Fig. 5a of XPS survey spectrum showed the signals of Bi, V, O and C elements have proved the existence of BCF composite. In the Bi 4f XPS spectra (Fig. 5b), pristine BVO presented two peaks at 159.3 eV and 164.6 eV were ascribed to Bi 4f7/2 and Bi 4f5/2 separately, which were corresponding to Bi ions in BVO [42,43]. In Fig. 5c, the peaks of pristine BVO at 516.9 eV and 524.3 eV were attributed to V 2p1/2 and V 2p3/2 and corresponding to V in BVO, respectively. For BCF composite, the peaks for Bi 4f showed two peaks at Bi 4f7/2 and Bi 4f5/2, respectively. The peaks for V 2p showed two peaks at V 2p1/2 and V 2p3/2, respectively [42,43]. The results demonstrated that BVO was growth on the natural fibers and no impurities in the BCF composite. For O 1s XPS spectra (Fig. 5d), an obvious shift to lower binding energy and new peaks were presented in BCF composite. The peaks at 529.8 eV and 530.6 eV were assigned to BieO and VeO, respectively. The new peak at 532.7 eV was belonged to OeH [44,45]. These changes were attributed to the chemical action between BVO and fiber, which was consistent with previous analysis of XRD, Raman and FT-IR that natural fibers could provide abundant combination bond.
where a, hn, A, Eg were absorption coefficient, incident photon energy, constant and band-gap. Thus, the band-gap of BCF was computed to be 2.23 eV, which could be excited under visible-light. The further photocatalytic experiments were confirmed that the BCF composite have a better visible light utilization.
Possible pathway of TC photodegradation The intermediates of TC were detected by LC-MS to further understand the process of degradation. The MS spectra and possible intermediates were presented in Figs. S2eS3. As
Please cite this article as: Wang T et al., In-situ synthesis of BiVO4 QDs/cellulose fibers composite for photocatalytic application, International Journal of Hydrogen Energy, https://doi.org/10.1016/j.ijhydene.2019.10.096
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Fig. 7 e UVevis spectra (a) and band gaps (b) of pure BiVO4 and BCF composite.
Fig. S2 showed the intensity peak of TC (m/z ¼ 445) was evident decreased, indicating the structure of TC was decomposed due to the active species [52]. For the TC molecules, the methyl groups were easily attacked by active species or happened dehydration reaction to form the molecules with m/z ¼ 434 and 378 (Fig. S3). Meanwhile, the product (m/ z ¼ 434) was continue to be decomposed to the new molecules with m/z ¼ 378, 304 and 338. As Fig. S3 showed the above intermediates (m/z ¼ 378, 304) would constantly lose the formyl groups, aldehyde group, carbonyl group and hydroxyl group [53,54] to product small molecules (m/z ¼ 356, 304, 269, 197, 136). These products were mineralized to inorganic ions and
molecules, indicating the BCF photocatalyst has the potential for the TC degradation.
Photocatalytic behavior and mechanism The main purpose of the material was designed to have good photocatalytic activity. The photocatalytic experiments were estimated by the degradation of TC solution under visiblelight irradiation. Before light illumination, all the samples were achieved the adsorption equilibrium under dark. As Fig. 8a showed, all the BCF composite exposed an increased photocatalytic activity than pure BVO QDs, which was
Fig. 8 e Photocatalytic experiments (a) and ln (C/C0)-t plots of different samples, trapping experiments (c) and cycle experiments (d) over BCF-3 composite. Please cite this article as: Wang T et al., In-situ synthesis of BiVO4 QDs/cellulose fibers composite for photocatalytic application, International Journal of Hydrogen Energy, https://doi.org/10.1016/j.ijhydene.2019.10.096
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Fig. 9 e Possible photocatalytic mechanism. attributed to the chemical bonds between BVO QDs and cellulose fiber to boost the electron transfer. The chemical link was more conducive to electrons migrate, due to the link played as an electronic bridge function. Among, the BCF-3 composite exhibited the optimum photocatalytic performance, indicating the ratio has a vital influence on the photocatalytic performance due to the appropriate active species [55]. To further rule out the adsorption process the photocatalytic test was performed on pure cellulose fibers. As the Fig. S4 showed the bare cellulose fibers achieved the adsorption equilibrium within 30 min and the adsorption capacity was about 10% under dark condition. Almost no photocatalytic activity for the pure bare cellulose fibers, which indicated the photocatalytic process played main role. The corresponding pseudo-first-order kinetics of degradation over all samples was presented in Fig. 8b, based on the calculated removal rate constants (K). The rate constant of BCF-3 composite (0.01233 min1) was 11.3 times higher than pure BVO QDs (0.00109 min1), demonstrating the photocatalytic activity of BVO QDs was greatly enhanced by chemical bonding of cellulose fiber. Moreover, the cycle experiments were carried out (Fig. 8c). After 3 times cycles of the experiment, the photocatalytic degradation over BCF-3 composite was still maintained, implying the composite has potential in practical applications. The mechanism investigations would help us better under the photocatalytic reaction process. It was generally recognized that trapping experiments were a method to analyze the active species during the catalytic process. The three main active species of hþ, ‧OH and O.2 were determined by the sacrificial agent CA, IPA and N2, respectively [56e58]. During the trapping experiments, the CA would deplete the hþ to judge whether the degradation effect changed. One situation that the degradation effect was not changed, indicating the hþ was not the main active species for the photocatalytic reaction (Fig. 8d). Another situation that the degradation effect
was significantly reduced, proving the hþ acted as a vital role in the photocatalytic process [59]. Identically, the function of ‧ þ OH and O.2 was demonstrated. As Fig. 8d showed, the h was the major active species during the photocatalytic process in this system, and ‧OH and O.2 have a small effect in the reaction process. Based on the above obtained results, a probable mechanism was mentioned (Fig. 9). The photocatalyst of BCF composite was excited by the visible-light illumination. Thus, the electron-hole pairs were produced in the BVO QDs and electrons could transfer to the cellulose fiber through the chemical connection. Therefore, the recombination opportunities of electrons and holes were greatly suppressed. This moment, the active species was reacted with pollutant to damage them and form a non-toxic small molecule.
Conclusions In a word, the biofiber was separated from bamboo, and the BVO QDs were successfully grown in the biofiber via in-situ growth. The BCF composite exhibited more efficient photocatalytic activity than pure BVO QDs to degrade TC solution under visible-light illumination. The increased photocatalytic property was attributed to the chemical bonding of fibers and BVO QDs, which not only increased the stability of BVO QDs in the cellulose fiber but also accelerated the electron transferences. The characterizes of FT-IR, XPS, Raman and XRD all demonstrated the BVO QDs was connected with the biofiber. Moreover, the active species trapping experiments were indicated the hþ was the major species for improving photocatalytic ability. The work provided a new insight for using biomaterials to design high-efficiency, simple, economical and green photocatalyst toward the environmental pollutant treatments.
Please cite this article as: Wang T et al., In-situ synthesis of BiVO4 QDs/cellulose fibers composite for photocatalytic application, International Journal of Hydrogen Energy, https://doi.org/10.1016/j.ijhydene.2019.10.096
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Acknowledgments The authors thank the financial support from the National Science Foundation of China (21908080, 21676115), Natural Science Foundation of Jiangsu Provincial (BK20180880, BK20180884), Postgraduate Research & Practice Innovation Program of Jiangsu Province (KYCX19_1621).
Appendix A. Supplementary data Supplementary data to this article can be found online at https://doi.org/10.1016/j.ijhydene.2019.10.096.
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Available online at www.sciencedirect.com
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In-situ synthesis of BiVO4 QDs/cellulose fibers composite for photocatalytic application Tao Wang a,d, Xiqing Liu b, Donglai Han d, Yuxuan Sun e, Changchang Ma c,d,**, Yang Liu d,f, Pengwei Huo c,d, Yongsheng Yan c,d,* a
School of the Environmental and Safety Engineering, Jiangsu University, 212013, Zhenjiang, PR China School of Material Science and Engineering, Jiangsu University, 212013, Zhenjiang, PR China c School of Chemistry and Chemical Engineering, Jiangsu University, 212013, Zhenjiang, PR China d Institute of Green Chemistry and Chemical Technology, Jiangsu University, 212013, Zhenjiang, PR China e College of Chemistry, Jilin Normal University, 13600, Siping, PR China f College of Physics, Jilin Normal University, 13600, Siping, PR China b
highlights
graphical abstract
Bamboo as the source to prepared cellulose fibers due to its abundant and short growth cycle. A novel BiVO4 QDs/fibers composite photocatalyst was obtained via the in-situ method. Rich groups of natural cellulose fibers provided many sites to form the
stability
and
distribution
BiVO4. The mechanism of synthesis and the photocatalytic process were discussed and proposed.
article info
abstract
Article history:
In this work, a biofiber was used as the natural polymer carrier to design a BiVO4 QDs/
Received 25 July 2019
cellulose fiber composite for photocatalytic application. The biofiber was obtained from
Received in revised form
bamboo, which was green, abundant and short growth cycle in Asia. Naturally rich
16 September 2019
groups of biofiber provided many sites to absorb the Bi3þ to form the uniform distribution
Accepted 12 October 2019
for BiVO4 QDs. Moreover, a series of results indicated the strong connection was formed
Available online xxx
between biofiber and BiVO4 QDs, which could increase the stability and electron transfer. Therefore, the new composite photocatalyst exhibited better stability and effectively
Keywords:
photocatalytic
activity.
Moreover,
the
possible
mechanism
of
synthesis
and
Biomaterials
* Corresponding author. School of Chemistry and Chemical Engineering, Jiangsu University, 212013, Zhenjiang, PR China. ** Corresponding author. E-mail addresses: [email protected] (C. Ma), [email protected] (Y. Yan). https://doi.org/10.1016/j.ijhydene.2019.10.096 0360-3199/© 2019 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved. Please cite this article as: Wang T et al., In-situ synthesis of BiVO4 QDs/cellulose fibers composite for photocatalytic application, International Journal of Hydrogen Energy, https://doi.org/10.1016/j.ijhydene.2019.10.096
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Natural cellulose fiber
photocatalytic were discussed, which provided insight for synthesizing photocatalytic
Chemical bonding
based on biomaterials.
Photocatalytic
© 2019 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.
BiVO4 QDs
Introduction Since the development of industrial, the growing pollution and destruction have caused serious problem [1e4]. Fortunately, new photocatalytic technology has been developed and it could apply in water splitting, CO2 conversion and organic removal via convert nature solar energy, thus attracting much attention [5e7]. Bismuth vanadium oxide (BiVO4, BVO) was one of newly photocatalytic material and possessed narrow bandgap, outstanding chemical stability, thus it has been known as a feasible visible-light-driven material [8e10]. Nevertheless, the common BVO has been limited by light response efficiency. Many researchers demonstrated that quantum-sized materials have widely investigated and applied in photoelectric devices, photocatalysis, and others due to their unique properties [11,12]. Therefore, many quantum sized semiconductor materials were developed and used in the photocatalytic fields, such as CdS, ZnO, ZnSe and so on [13e15]. As expected, quantum-sized BVO has prepared and Sun et al. making it be a photocatalyst for H2 evolution due to quantum confinement effect [16]. Unfortunately, quantum-sized materials are easily to aggregate because of high surface energy, resulted in poor stability and low catalytic activity. Generally speaking, constructing composite photocatalyst could increase the stability of quantum sized materials [17]. Meanwhile, composite photocatalyst would exhibit better catalytic activity than pristine material [18,19]. For example, Wang's group reported that vanadate quantum dots (QDs) interspersed g-C3N4 could enhance efficient inactivation of Salmonella via absorbing light source [20]. Li et al. reported a BVO QDs decorated BiPO4 nanorods via in-situ growth method, which also increased visible-light-driven photocatalytic activity [21]. Luo et al. designed a CuInS2 QDs/BiWO6 photocatalyst, resulting in higher photocatalytic activity due to the configuration of p-n heterojunction and simultaneously tune the behavior of photogenerated charge carriers [22]. An ideal substrate for BVO QDs, efficient and environmentally friendly, should be developed. Cellulose, one of the most abundant biopolymer on Earth, which has appealing mechanical properties, special modulus and special strength [23,24]. Among, bamboo fiber was the main natural source of cellulose and widely distributed in Asia. Bamboo, an ideal source of cellulose fiber (CF) due to their preponderance of the breeding fast, good renewability, high yield, wide-ranging and environmentally friendly [25e27]. Cellulose, the structure of the superfine network not only provides mechanical support but also benefit to disperse the nanoparticles and enhance the photocatalyst stability. In addition, the hydroxyl groups in the cellulose structure could
connect with semiconductor oxide particles. Some reports have demonstrated that the semiconductor oxide particles into a cellulose polymer matrix showed enhanced properties. For example, Mohamed M.A. et al. incorporated NeTiO2 nanorods in cellulose membrane matrix, forming a strong interaction between the hydroxyl groups of cellulose and TiO2 through bonding interactions [28]. In this work, the novel BVO QDs/nature cellulose fiber composite were obtained through in situ growth method under ultrasound with use of bamboo as the cellulose source. The formation process of BVO QDs decorated on cellulose fiber and the possible bonding effect was discussed. The physicochemical characteristic of BVO-cellulose fiber composite was studied. Moreover, the photocatalytic performance of BVOcellulose fiber composite was determined by the degradation of the organic pollutant aqueous solution. As a result, the stability of BVO QDs was enhanced via the interaction with hydroxyl groups of cellulose, and the charge carrier transfer on the BVO-cellulose fiber resulted in improved the photocatalytic activity. The crystal structure, photocatalytic mechanism, chemical groups of the BVO-cellulose fiber composite were studied for open up a simple, effective and economic strategy toward the design of unique nature cellulose-based materials, which may provide a practical visible-light photocatalyst.
Experimental Chemicals Bamboo from Jiangsu University campus. Bismuth nitrate pentahydrate (Bi(NO3)3‧5H2O), ammonium metavanadate (NH4VO3), sodium sulfite (Na2SO3) tetracycline (TC) and citric acid monohydrate (C6H8O7‧H2O, CA) were obtained from Aladdin chemistry Co. Ltd (Shanghai, China). Ammonia solution (NH3H2O), ethanol (C2H5OH), isopropyl alcohol (C3H7OH, IPA), hydrogen peroxide solution (H2O2) and sodium hydroxide (NaOH) were purchased from Sinopharm Chemical Reagent Co., Ltd (Shanghai, China). All reagents were all of the analytic grades and used without a further treat. The deionized water used throughout the whole experiment.
Natural cellulose fiber obtained from bamboo As we known, bamboo stems were mainly composed of cellulose, hemicellulose, lignin and other chemicals. Thus, it was necessary to gradually remove other components except for cellulose. The bamboo cut into small species and washed for the following treatment. The mixed solution was consisted of by dissolving NaOH (2.5 M) and Na2SO3 (0.4 M) in deionized
Please cite this article as: Wang T et al., In-situ synthesis of BiVO4 QDs/cellulose fibers composite for photocatalytic application, International Journal of Hydrogen Energy, https://doi.org/10.1016/j.ijhydene.2019.10.096
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water. The bamboo species was immersed in the mixed solution and kept boiling for 24 h, followed by rinsing in deionized water to remove the chemicals. Then, the bamboo species were placed in the 2.5 M H2O2 solution for boiling without stirring. When the green bamboo changed to white, the sample was filtered and washed with deionized water. The cellulose was obtained from the above process, and drying for further experiments.
The preparation of BiVO4 quantum dots/cellulose fiber composite The composite was prepared via a simply in suit ultrasonic method. Firstly, the cellulose fiber was added into Bi(NO3)3‧ 5H2O (30 mL, 5 mM) solution under ultrasound to form a uniform suspension. Then, the NH4VO3 solution (30 mL, 5 mM) was added into the suspension solution with strongly stirring and ultrasound. Next, the pH of the solution was adjusted to 7 with NH3‧H2O solution. The obtained precipitates were centrifugation, washed with deionized water and ethanol, and dried at low temperature. The pure vanadate QDs was synthesized by the same process without added cellulose fiber. The theoretical weight ration of cellulose fiber in the BiVO4 QDs/cellulose fiber was 15 wt%, 10 wt%, 5 wt% and 1 wt%, the corresponding samples were marked as BCF-1, BCF-2, BCF-3 and BCF-4, respectively.
Photocatalytic experiment The photocatalytic performance of BCF composite was determined by the degradation and 300 W Xe lamp (cut off 420 nm) as the light source. The photocatalyst (20 mg) was dispersed in 100 mL 10 mg/L TC solution by violent stirring to achieve an adsorption-desorption equilibrium under dark conditions. Then, the suspension was exposed to light illumination with stirring. At each time interval, 4 mL of suspension was collected to remove the photocatalyst, and the absorption of TC solution was applied to analyze its degradation by UV-2700 spectrophotometer.
Material characterization The crystal structure of the samples was determined by X-ray diffraction (XRD). The morphology of samples was observed by field-emission electron microscope (FE-SEM), and the
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elemental distribution of composite was analyzed by corresponding SEM with X-ray energy dispersive spectroscopy (EDS). Fourier transform infrared spectra (FT-IR) was used to decide the chemical groups. The surface chemical analyses of the sample were carried out by X-ray photoelectron spectroscopy (XPS). The Brunauer-Emmett-Teller (BET) surface areas of prepared samples were determined via N2 adsorption isotherms. Further structural was analyzed by Raman spectroscopy. The optical absorption spectra and diffuse reflection spectra were analyzed by UVevis spectrophotometer with an integrating sphere.
Results and discussion The formation process of BiVO4 QDs-cellulose fibers The preparation process and possible mechanism of BVO QDs loaded on cellulose fiber were proposed (Fig. 1). The support of cellulose fiber was obtained from bamboo through removing lignin and other ingredients. Due to sufficient hydroxy and carboxyl on the molecule chain of cellulose fiber, which provided many sites for adsorbing Bi3þ [29,30]. The BVO was started to crystallize when added the NH4VO3 solution. In order to inhibit the agglomeration by rapid crystallization of BiVO4, the reaction was kept strong stirring and ultrasound. Finally, the reaction was completed to achieve a quantum size BVO growth on the surface of cellulose fiber. During the reaction, the sufficient hydroxy and carboxyl not only provided the sites for the growth of BVO QDs but also could increase the stability of composite due to chemical adsorbed.
Morphology and structure analysis As Fig. 2a showed, the cellulose fiber was like a very long line, which exhibited irregular size and micron length due to the uncontrollability of biological materials [31]. These would provide enough area for the growth of BVO QDs. The SEM image of BCF composite was presented in Fig. 2b, the surface of cellulose fiber changed rough. As observed, the rough surface consisted of much nanoparticles, which may be attributed to the BVO QDs were growth in the surface of cellulose fiber [32]. In addition, the TEM images were further to observe the morphology of BCF composite. As Fig. S1a showed much nanoparticles were loaded on the surface of large fiber. The
Fig. 1 e The possible synthesis mechanism of BCF composite. Please cite this article as: Wang T et al., In-situ synthesis of BiVO4 QDs/cellulose fibers composite for photocatalytic application, International Journal of Hydrogen Energy, https://doi.org/10.1016/j.ijhydene.2019.10.096
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Fig. 2 e The SEM images of natural bamboo fibers (a) and BCF composite (b), corresponding EDS mapping (cee).
Fig. 3 e XRD patterns (a) and enlarged XRD patterns (b) of pure BiVO4 and BCF composite.
nanoparticles were ascribed to BVO QDs with the size about 10 nm, which was consistent with the SEM images. Moreover, the lattice fringe at 0.48 nm was attributed to the d-spacing of (110) of BVO (Fig. S1b), further confirming the formation of BVO QDs on fibers. Meanwhile, the corresponding EDS mapping of BCF composite further demonstrated that the BVO QDs were evenly dispersed on the apparent of cellulose fiber, which contained elements of Bi, V and O. Further verifying the BVO QDs was successfully synthesized, some characterizations were adopted. The crystal structures of prepared materials were tested via the XRD, shown in Fig. 3a. It clearly found that the diffraction peaks of BVO QDs were fully corresponding to the BVO standard card (PDF#44-0081). The intensity peaks of BVO QDs indicated that the sample has good crystallinity without impurity [33]. For the BCF composite, the diffraction peaks were still corresponding to the BVO, implying the BVO QDs
maintained the BVO crystal structure in the composite material. However, no peaks belonged to cellulose fiber, which may be attributed to the low crystallinity formed by complex organic structures. In the enlarged XRD spectra (Fig. 3b), an obviously shifted was happed in the BCF composite compared to pure BVO QDs. The changes would demonstrate the BVO QDs were growth in the cellulose fiber and were consistent with the above analysis that Bi3þ connected cellulose fiber with chemical bonding [34]. The analysis was further verified by the following examination. Raman spectroscopy was applied to study the BVO QDs’ vibrational properties and structural, the spectra were presented in Fig. 4a. For the pure BVO QDs, the intense peak at 829 cm1 was ascribed to symmetric VeO stretching mode and a weak shoulder at about 708 cm1 ascribed to asymmetric VeO stretching mode. The peaks located at about 325 and 367 cm1 were attributed to the symmetric bending mode
Please cite this article as: Wang T et al., In-situ synthesis of BiVO4 QDs/cellulose fibers composite for photocatalytic application, International Journal of Hydrogen Energy, https://doi.org/10.1016/j.ijhydene.2019.10.096
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Fig. 4 e Raman (a) and FT-IR (b) of samples.
and the asymmetric bending of vanadate anions, respectively [35,36]. Moreover, the external modes (rotation/translation) were appeared at about 127 and 211 cm1, respectively [37,38]. The result further verified the BVO QDs was prepared. For the Raman spectra of BCF composite, the peaks maintained the features of BVO QDs obviously. However, the intensity and position of peaks were changed in the BCF composite compared to pure BVO QDs, which demonstrated the BVO QDs growth in cellulose fiber with the connection of hydroxy and carboxyl. The changed of chemical groups was determined by FT-IR, which could prove the chemical interaction between BVO QDs and cellulose fiber. For pure BVO QDs, the vibration band
located at 679 cm1 could be ascribed to the asymmetric stretching vibration of the VO4 [39]. For pure cellulose fiber, the hydroxyl and carboxyl groups were detected. The peaks characterization at about 615, 1059, 1376, 1594, 2897, 2794 and 3366 cm1, were assigned to the CH2, CeOeC, C]O, CH3, CH2 and OeH, respectively [40,41]. It clearly found that primary bands of BVO QDs and cellulose fiber were included in composite, indicating the BCF composite were prepared successfully. Moreover, the peaks of chemical groups in the BCF composite were disappeared or displacement, which proved a bond connection was formed between BVO and cellulose fiber. The chemical bond would increase the stability and charge transfer of BCF composite.
Fig. 5 e XPS spectra of BVO and BCF composite, (a) survey, (b) Bi 4f, (c) V 2p and (d) O 1s. Please cite this article as: Wang T et al., In-situ synthesis of BiVO4 QDs/cellulose fibers composite for photocatalytic application, International Journal of Hydrogen Energy, https://doi.org/10.1016/j.ijhydene.2019.10.096
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Fig. 6 e N2 adsorption-desorption isotherms of BVO, cellulose fibers and BCF composite (a), Nyquist plot of BVO and BCF composite (b).
BET analysis The BET surface area of the samples was obtained by N2 adsorption-desorption isotherms [46]. As Fig. 6a showed all samples displayed a type hysteresis loop in type-III isotherm, indicating that the material did not have pores or have large pores. The results were consistent with the SEM images. According to the computer, the BET surface area of cellulose fiber, BVO QDs and BCF were 78.935, 62.561 and 29.835 m2/g, respectively. The large surface area of cellulose fiber would provide enough sites for the growth of BVO QDs. As expected, the surface area of BCF was smaller than the pure CF, indicating the BVO QDs were growth in the cellulose fiber. Generally speaking, the larger surface area would benefit to the photocatalytic activity [47]. But in this work, the BCF composite displayed better catalytic activity than pure BVO QDs, which surface area of BCF was smaller than BVO QDs, demonstrating that the electronic transfer played the main
role in the composite instead of pure materials. The better electronic transfer may be attributed to the chemical connection between cellulose fiber and BVO QDs. Thus, the electrochemical impedance spectroscopy was used to demonstrate the charge transfer abilities of the samples based on the charge transfer resistance. As general, the smaller radius size of the Nyquist plot implied the better change transfer due to the small the charge transfer resistance. From the Fig. 6b, the radius of BCF composite was smaller than pure BVO, revealing the high charge transfer rate for improving photocatalytic activity.
Optical properties The light absorption properties were an important indicator for determining whether the materials were excited by visible light [48e50], the UVevis DRS spectra were presented in Fig. 7. Obviously, the absorption edge of BCF composite was more than 500 nm, indicating the BCF composite could be excited under visible-light. However, the absorption wavelength region of BCF composite showed slight red-shift compare to pristine BVO QDs, which was attributed to the color of the cellulose fiber was white. It was worth noting that the absorbance intensity of BCF composite was increased, which was attributed to the C]C and C]O bands. Moreover, the bandgap energy of samples could be calculated through the formula [51]: 1 2
ahn ¼ Aðhn Eg Þ
=
The surface chemical state and chemical link of the BCF composite, the pure BVO and BCF composite were studied via XPS measurement. As Fig. 5a of XPS survey spectrum showed the signals of Bi, V, O and C elements have proved the existence of BCF composite. In the Bi 4f XPS spectra (Fig. 5b), pristine BVO presented two peaks at 159.3 eV and 164.6 eV were ascribed to Bi 4f7/2 and Bi 4f5/2 separately, which were corresponding to Bi ions in BVO [42,43]. In Fig. 5c, the peaks of pristine BVO at 516.9 eV and 524.3 eV were attributed to V 2p1/2 and V 2p3/2 and corresponding to V in BVO, respectively. For BCF composite, the peaks for Bi 4f showed two peaks at Bi 4f7/2 and Bi 4f5/2, respectively. The peaks for V 2p showed two peaks at V 2p1/2 and V 2p3/2, respectively [42,43]. The results demonstrated that BVO was growth on the natural fibers and no impurities in the BCF composite. For O 1s XPS spectra (Fig. 5d), an obvious shift to lower binding energy and new peaks were presented in BCF composite. The peaks at 529.8 eV and 530.6 eV were assigned to BieO and VeO, respectively. The new peak at 532.7 eV was belonged to OeH [44,45]. These changes were attributed to the chemical action between BVO and fiber, which was consistent with previous analysis of XRD, Raman and FT-IR that natural fibers could provide abundant combination bond.
where a, hn, A, Eg were absorption coefficient, incident photon energy, constant and band-gap. Thus, the band-gap of BCF was computed to be 2.23 eV, which could be excited under visible-light. The further photocatalytic experiments were confirmed that the BCF composite have a better visible light utilization.
Possible pathway of TC photodegradation The intermediates of TC were detected by LC-MS to further understand the process of degradation. The MS spectra and possible intermediates were presented in Figs. S2eS3. As
Please cite this article as: Wang T et al., In-situ synthesis of BiVO4 QDs/cellulose fibers composite for photocatalytic application, International Journal of Hydrogen Energy, https://doi.org/10.1016/j.ijhydene.2019.10.096
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Fig. 7 e UVevis spectra (a) and band gaps (b) of pure BiVO4 and BCF composite.
Fig. S2 showed the intensity peak of TC (m/z ¼ 445) was evident decreased, indicating the structure of TC was decomposed due to the active species [52]. For the TC molecules, the methyl groups were easily attacked by active species or happened dehydration reaction to form the molecules with m/z ¼ 434 and 378 (Fig. S3). Meanwhile, the product (m/ z ¼ 434) was continue to be decomposed to the new molecules with m/z ¼ 378, 304 and 338. As Fig. S3 showed the above intermediates (m/z ¼ 378, 304) would constantly lose the formyl groups, aldehyde group, carbonyl group and hydroxyl group [53,54] to product small molecules (m/z ¼ 356, 304, 269, 197, 136). These products were mineralized to inorganic ions and
molecules, indicating the BCF photocatalyst has the potential for the TC degradation.
Photocatalytic behavior and mechanism The main purpose of the material was designed to have good photocatalytic activity. The photocatalytic experiments were estimated by the degradation of TC solution under visiblelight irradiation. Before light illumination, all the samples were achieved the adsorption equilibrium under dark. As Fig. 8a showed, all the BCF composite exposed an increased photocatalytic activity than pure BVO QDs, which was
Fig. 8 e Photocatalytic experiments (a) and ln (C/C0)-t plots of different samples, trapping experiments (c) and cycle experiments (d) over BCF-3 composite. Please cite this article as: Wang T et al., In-situ synthesis of BiVO4 QDs/cellulose fibers composite for photocatalytic application, International Journal of Hydrogen Energy, https://doi.org/10.1016/j.ijhydene.2019.10.096
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Fig. 9 e Possible photocatalytic mechanism. attributed to the chemical bonds between BVO QDs and cellulose fiber to boost the electron transfer. The chemical link was more conducive to electrons migrate, due to the link played as an electronic bridge function. Among, the BCF-3 composite exhibited the optimum photocatalytic performance, indicating the ratio has a vital influence on the photocatalytic performance due to the appropriate active species [55]. To further rule out the adsorption process the photocatalytic test was performed on pure cellulose fibers. As the Fig. S4 showed the bare cellulose fibers achieved the adsorption equilibrium within 30 min and the adsorption capacity was about 10% under dark condition. Almost no photocatalytic activity for the pure bare cellulose fibers, which indicated the photocatalytic process played main role. The corresponding pseudo-first-order kinetics of degradation over all samples was presented in Fig. 8b, based on the calculated removal rate constants (K). The rate constant of BCF-3 composite (0.01233 min1) was 11.3 times higher than pure BVO QDs (0.00109 min1), demonstrating the photocatalytic activity of BVO QDs was greatly enhanced by chemical bonding of cellulose fiber. Moreover, the cycle experiments were carried out (Fig. 8c). After 3 times cycles of the experiment, the photocatalytic degradation over BCF-3 composite was still maintained, implying the composite has potential in practical applications. The mechanism investigations would help us better under the photocatalytic reaction process. It was generally recognized that trapping experiments were a method to analyze the active species during the catalytic process. The three main active species of hþ, ‧OH and O.2 were determined by the sacrificial agent CA, IPA and N2, respectively [56e58]. During the trapping experiments, the CA would deplete the hþ to judge whether the degradation effect changed. One situation that the degradation effect was not changed, indicating the hþ was not the main active species for the photocatalytic reaction (Fig. 8d). Another situation that the degradation effect
was significantly reduced, proving the hþ acted as a vital role in the photocatalytic process [59]. Identically, the function of ‧ þ OH and O.2 was demonstrated. As Fig. 8d showed, the h was the major active species during the photocatalytic process in this system, and ‧OH and O.2 have a small effect in the reaction process. Based on the above obtained results, a probable mechanism was mentioned (Fig. 9). The photocatalyst of BCF composite was excited by the visible-light illumination. Thus, the electron-hole pairs were produced in the BVO QDs and electrons could transfer to the cellulose fiber through the chemical connection. Therefore, the recombination opportunities of electrons and holes were greatly suppressed. This moment, the active species was reacted with pollutant to damage them and form a non-toxic small molecule.
Conclusions In a word, the biofiber was separated from bamboo, and the BVO QDs were successfully grown in the biofiber via in-situ growth. The BCF composite exhibited more efficient photocatalytic activity than pure BVO QDs to degrade TC solution under visible-light illumination. The increased photocatalytic property was attributed to the chemical bonding of fibers and BVO QDs, which not only increased the stability of BVO QDs in the cellulose fiber but also accelerated the electron transferences. The characterizes of FT-IR, XPS, Raman and XRD all demonstrated the BVO QDs was connected with the biofiber. Moreover, the active species trapping experiments were indicated the hþ was the major species for improving photocatalytic ability. The work provided a new insight for using biomaterials to design high-efficiency, simple, economical and green photocatalyst toward the environmental pollutant treatments.
Please cite this article as: Wang T et al., In-situ synthesis of BiVO4 QDs/cellulose fibers composite for photocatalytic application, International Journal of Hydrogen Energy, https://doi.org/10.1016/j.ijhydene.2019.10.096
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Acknowledgments The authors thank the financial support from the National Science Foundation of China (21908080, 21676115), Natural Science Foundation of Jiangsu Provincial (BK20180880, BK20180884), Postgraduate Research & Practice Innovation Program of Jiangsu Province (KYCX19_1621).
Appendix A. Supplementary data Supplementary data to this article can be found online at https://doi.org/10.1016/j.ijhydene.2019.10.096.
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Please cite this article as: Wang T et al., In-situ synthesis of BiVO4 QDs/cellulose fibers composite for photocatalytic application, International Journal of Hydrogen Energy, https://doi.org/10.1016/j.ijhydene.2019.10.096