APPLIED SURFACE SCIENCE
·
2017
·
IF 3.387
Wei Jiang,Zhaomei Wu,Yingming Zhu,Wen Tian,Bin Liang
Four silver chalcogen compounds, Ag 2 O, Ag 2 S, Ag 2 Se and Ag 2 Te, can be utilized as visible-light-driven photocatalysts. In this research, the electronic structures of these compounds were analyzed by simulation and experiments to systematically reveal the relationship between photocatalytic performance and energetic structure. All four chalcogenides exhibited interesting photocatalytic activities under ultraviolet, visible and near-infrared light. However, their photocatalytic performances and stability significantly depended on the band gap width, and the valence band and conduct band position, which was determined by their composition. Increasing the X atomic number from O to Te resulted in the upward movement of the valence band top and the conduct band bottom, which resulted in narrower band gaps, a wider absorption spectrum, a weaker photo-oxidization capacity, a higher recombination probability of hole and electron pairs, lower quantum efficiency, and worse stability. Among them, Ag 2 O has the highest photocatalytic performance and stability due to its widest band gap and lowest position of VB and CB. The combined action of photogenerated holes and different radicals, depending on the different electronic structures, including anion ozone radical, hydroxide radical, and superoxide radical, was observed and understood. The results of experimental observations and simulations of the four silver chalcogen compounds suggested that a proper electronic structure is necessary to obtain a balance between photocatalytic performance and absorbable light region in the development of new photocatalysts.
研究领域:
材料科学
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化学
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DOI
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-11
·
IF 15.7
Wang Zhouzhou,Ye Haotian,Li Yixin,Sheng Bowen,Wang Ping,Ou Pengfei,Li Xiao-Yan,Yu Tianqi,Huang Zijian,Li Jinglin,Yu Ying,Wang Xinqiang,Huang Zhen,Zhou Baowen
Light-driven bioethanol dehydration offers attractive outlooks for the sustainable production of ethylene. Herein, a surface-hydrogenated CrMnO x is coupled with GaN nanowires (GaN@CMO-H) for light-driven ethanol dehydration to ethylene. Through combined experimental and computational investigations, a surface hydrogen-replenishment mechanism is proposed to disclose the ethanol dehydration pathway over GaN@CMO-H. Moreover, the surface-hydrogenated GaN@CMO-H can significantly lower the reaction energy barrier of the C 2 H 5 OH-to-C 2 H 4 conversion by switching the rate-determining reaction step compared to both GaN and GaN@CMO. Consequently, the surface-hydrogenated GaN@CMO-H illustrates a considerable ethylene production activity of 1.78 mol·g cat −1 ·h −1 with a high turnover number of 94,769 mole ethylene per mole CrMnO x . This work illustrates a new route for sustainable ethylene production with the only use of bioethanol and sunlight beyond fossil fuels.
研究领域:
材料科学
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催化化学
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可持续能源
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Crystals
·
2023
·Vol. 13
·期 11
·1531
·
IF 2.7
Li Wang,Junbo Wang,Yanfei Fei,Heping Cheng,Hua Pan,Chunfeng Wu
Novel Ag3PO4/Bi2WO6catalysts with enhanced visible-light performance were synthesized using a hydrothermal method and characterized to investigate their morphology, microscopic structure, and binding energies. Photoluminescence spectrum (PL) and electrochemical impedance spectroscopy (EIS) data demonstrate that the formed Ag3PO4/Bi2WO6heterojunction effectively promotes hole (h+)–electron (e−) separation and transfer efficiency, resulting in the enhancement of photocatalytic activity. Ag3PO4/Bi2WO6displays higher photocatalytic activity than pure Bi2WO6or Ag3PO4alone. Photogenerated holes (h+), ·O2−, and ·OH were found to be the main active species for the degradation of malachite green (MG), methylene blue (MB), and Rhodamine B (RhB). The DFT calculation explains the photostability of Ag3PO4/Bi2WO6from the perspective of electronic structure. The bandgap of Ag3PO4/Bi2WO6between the highest occupied molecular orbital (HOMO) and the lowest unoccupied molecular orbital (LUMO) is 1.41 eV, compared with that of Ag3PO4at 0.91 eV and Bi2WO6at 2.59 eV. Ag–O–Bi hybridization and the wide HOMO–LUMO bandgap lead to difficulty in electron transfer. As a consequence, Ag+is difficult to obtain electrons and difficult to convert into Ag0, which makes the catalyst stable.Keywords:Ag3PO4;Bi2WO6;heterojunction;photocatalyst;visible-light-driven
研究领域:
材料科学
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环境科学
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化学
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产品关联
DOI
高影响因子
Nature Chemistry
·
2024
·Vol. 16
·期 3
·373-379
·
IF 19.2
Guan Yeqin,Wen Hong,Cui Kaixun,Wang Qianru,Gao Wenbo,Cai Yongli,Cheng Zibo,Pei Qijun,Li Zhao,Cao Hujun,He Teng,Guo Jianping,Chen Ping
Photon-driven chemical processes are usually mediated by oxides, nitrides and sulfides whose photo-conversion efficiency is limited by charge carrier recombination. Here we show that lithium hydride undergoes photolysis upon ultraviolet illumination to yield long-lived photon-generated electrons residing in hydrogen vacancies, known as F centres. We demonstrate that photon-driven dehydrogenation and dark rehydrogenation over lithium hydride can be fulfilled reversibly at room temperature, which is about 600 K lower than the corresponding thermal process. As light-driven F centre generation could provide an alternative approach to charge carrier separation to favour chemical transformations that are kinetically or thermodynamically challenging, we show that light-activated lithium hydride cleaves the N≡N triple bond to form a N–H bond under mild conditions. Co-feeding a N 2 /H 2 mixture with low H 2 partial pressure leads to photocatalytic ammonia formation at near ambient conditions. This work provides insights into the development of advanced materials and processes for light harvesting and conversion.
研究领域:
化学
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材料科学
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催化
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光化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Mei Cai,Bin Du,Anze Shui,Chao He
The photodegradation of pollutants is a significant and friendly technology to protect the environment. The fabrication of hierarchical heterojunction is the efficient method to improve the photocatalytic performance. Herein, the hierarchical type-II BiOBr@ZnIn 2 S 4 heterojunction is fabricated successfully via a simple chemistry method. The optimal sample BS170 (the volume of 170 mL ethylene glycol) exhibits the higher photodegradation under the visible light and presents 2.3 times higher than that of pure BiOBr for degradation of MO and the mass of BS170 is the half of BiOBr could achieve the same photocatalytic effect as BiOBr for the photodegradation of RhB. The results indicate the fabric of heterojunction could enhance the absorption capacity of visible light and separation efficiency of photoinduced electron-hole pairs to increase the photodegradation. Therefore, this work provides the novel strategy for fabricating the hierarchical type-II heterojunction photocatalyst for the degradation of dyes.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
·
2017
·Vol. 2017
·期 40
·4797-4802
·
IF 2.444
Yulan Peng,Lingzhi Wang,Yongdi Liu,Haijun Chen,Juying Lei,Jinlong Zhang
Graphical A CoP-decorated g-C 3 N 4 composite catalyst was developed for highly efficient and stable photocatalytic production of H 2 O 2 under visible-light irradiation. The CoP nanoparticles act as a noble metal free cocatalyst for g-C 3 N 4 to enhance the visible-light absorption and promote the separation of photogenerated charge carriers. A composite catalyst combining CoP with g-C 3 N 4 was explored for the photocatalytic production of H 2 O 2 under visible-light irradiation. The composite catalyst was fabricated by growth of CoP nanoparticles on the surface of g-C 3 N 4 . The CoP nanoparticles were well dispersed on the surface of g-C 3 N 4 and could interact with g-C 3 N 4 to improve charge separation and electron transfer. The composite catalyst showed superior catalytic activity compared with pure CoP or g-C 3 N 4 under visible-light irradiation. The optimal catalyst with 1.76 wt.-% CoP loading exhibited the best photocatalytic efficiency with an H 2 O 2 production of 140 µ m in 2 h, which is about 4.6 and 23.3 times those of pure g-C 3 N 4 and pure CoP, respectively. A possible mechanism for the visible-light-driven photocatalytic production of H 2 O 2 is proposed. The composite catalyst exhibited stable performance without obvious loss of catalytic activity after seven successive runs, and thus has good application prospects in sustainable H 2 O 2 production.
研究领域:
材料科学
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环境科学
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化学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2021
·
IF 5.816
Xu Yang,Zhaoxia Zhang,Xiaoyang Wang,Guanghua Wang,Xinlong Tian,Zhifu Wu
Overcoming the limited light harvest and sluggish charge transfer efficiency has remained a long-standing challenge for the practical application of visible-light driven hydrogen evolution . In this work, a novel cobalt doped titanium nitride interlaced nanotube was synthesized through a facile hydrothermal approach and subsequent ammonia gas nitrification route. The optimized Ti 0·75 Co 0·25 N (molar ratio of Ti:Co:N = 0.75:0.25:1) catalyst delivered the highest hydrogen yield in visible-light-induced water splitting, which was almost 2 times higher than the pristine TiN did. Further structure characterizations have unraveled that the cobalt atoms were partially substituted the titanium atoms in crystallite lattice, generating a significant synergistic regulation on band structure and electronic state. As a result, the narrowed energy bandgap, improved charge carrier mobility and lowered over-potential contributed to the high electron-hole separation efficiency and smoothed interface charge transfer, yielding an enhanced photocatalytic activity . This work is a significant contribution to the design of efficient and stable visible light driven water splitting catalysts.
研究领域:
材料科学
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催化化学
✓ 已验证
DOI
高影响因子
Journal of the American Chemical Society
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2020
·
IF 14.612
Peishen Li,Ziang Zhou,Qiang Wang,Ming Guo,Shaowei Chen,Jingxiang Low,Ran Long,Wen Liu,Peiren Ding,Yunyun Wu,Yujie Xiong
Photocatalytic nitrogen fixation represents a green alternative to the conventional Haber–Bosch process in the conversion of nitrogen to ammonia. In this study, a series of Bi5O7Br nanostructures were synthesized via a facile, low-temperature thermal treatment procedure, and their photocatalytic activity toward nitrogen fixation was evaluated and compared. Spectroscopic measurements showed that the tubular Bi5O7Br sample prepared at 40 °C (Bi5O7Br-40) exhibited the highest electron-transfer rate among the series, producing a large number of O2.– radicals and oxygen vacancies under visible-light photoirradiation and reaching a rate of photocatalytic nitrogen fixation of 12.72 mM·g–1·h–1 after 30 min of photoirradiation. The reaction dynamics was also monitored by in situ infrared measurements with a synchrotron radiation light source, where the transient difference between signals in the dark and under photoirradiation was analyzed and the reaction pathway of nitrogen fixation was identified. This was further supported by results from density functional theory calculations. The reaction energy of nitrogen fixation was quantitatively estimated and compared by building oxygen-enriched and anoxic models, where the change in the oxygen vacancy concentration was found to play a critical role in determining the nitrogen fixation performance. Results from this study suggest that Bi5O7Br with rich oxygen vacancies can be used as a high-performance photocatalyst for nitrogen fixation.
研究领域:
材料科学
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环境科学
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催化化学
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DOI
PubMed
高影响因子
JOURNAL OF MATERIALS SCIENCE
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2022
·Vol. 57
·期 6
·4092-4103
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IF 4.682
Chen Zongchen,Jiang Jiwei,Wang Xin,Zhang Hui,Song Bo,Dong Bin
Inspired by the swarming behavior of various bacteria in nature, light-driven micromotor with collective behavior has attracted a great deal of attention, which will be a valuable tool to understand the cooperation and communication between bacterial populations and will contribute to the creation of reconfigurable microrobots and the cooperative transportation of large cargoes. However, it is still challenging to modulate the micromotors’ collective behavior based on local interaction and communication. Herein, we develop a light-powered BiVO 4 -based micromotor with self-propulsion and dynamic ‘predator-bait’ collective behavior, which is based on the photocatalytic reaction of BiVO 4 . The BiVO 4 -based micromotor has great potential in the field of organic pollutant degradation with enhanced apparent rate constant (0.076 min −1 ) which originates from the dynamic ‘predator-bait’ behavior.
研究领域:
材料科学
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环境科学
·
仿生学
✓ 已验证
DOI
高影响因子
MATERIALS CHARACTERIZATION
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2020
·
IF 3.562
Xiaoxia Guo,Dan Wu,Xia Long,Zihan Zhang,Fenglin Wang,Guanghua Ai,Xiaohe Liu
The nanosheet-assembled Bi 2 WO 6 microspheres could be successfully synthesized in large quantities by a facile hydrothermal strategy in the presence of surfactant hexadecyl trimethyl ammonium bromide (CTAB) and polyvinylpyrrolidone (PVP) under mild conditions. The morphology and size of as-prepared Bi 2 WO 6 could be readily controlled by adjusting the synthetic parameters such as hydrothermal time. The probable formation mechanism of nanosheet-assembled Bi 2 WO 6 microspheres was discussed in detail. The hierarchical nanosheet-assembled microspheres could be constructed by orderly arranged nanosheets. The photocatalytic activity of the nanosheet-assembled Bi 2 WO 6 microspheres was evaluated by degrading rhodamine B (RhB) under irradiation of visible light. The brilliant photodegradation efficiency is about 98% under visible light irradiation for 50 min. The results suggest that the as-prepared Bi 2 WO 6 microspheres have good prospects as the photocatalyst for the removal of organic pollutants .
研究领域:
材料科学
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环境科学
✓ 已验证
DOI
高影响因子
JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
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2020
·
IF 3.306
Shuguang Li,Zhiyu Liu,Chunxiao Lu,Zhihui Qu,Congcong Piao,Jianhe Tang,Dawei Fang,Jun Wang
The use of co-catalysts can observably enhance photocatalytic hydrogen production activity. In this work, a novel visible-light driven photocatalyst, (MoSe 2 -RGO)/(Er 3+ :Y 3 Al 5 O 12 /ZnS)/RuO 2 nanocomposite, is prepared for the first time by loading Er 3+ :Y 3 Al 5 O 12 , MoSe 2 -RGO and RuO 2 on the surface of ZnS nanoparticles. Er 3+ :Y 3 Al 5 O 12 as an effective visible-to-ultraviolet up-conversion luminescence agent can provide the ultraviolet-light to activate wide band-gap ZnS. MoSe 2 -RGO and RuO 2 , acting as conduction band co-catalyst and valence band co-catalyst, respectively, can effectively separate the photo-generated carriers and supply more reactive sites. The activities of the photocatalysts were assessed via photocatalytic hydrogen production in Na 2 S and Na 2 SO 3 aqueous solution under 300 W xenon lamp irradiation. In addition, the visible-light irradiation time and used times of the prepared samples as influence factors on the photocatalytic hydrogen production were also investigated. It was easily found that the prepared (MoSe 2 -RGO)/(Er 3+ :Y 3 Al 5 O 12 /ZnS)/RuO 2 nanocomposite shows fairly high activity in photocatalytic hydrogen production, compared with single ZnS photocatalyst. It was mainly attributed to the excellent up-conversion luminescence property of Er 3+ :Y 3 Al 5 O 12 and the efficient separation of photo-generated electrons and holes caused by MoSe 2 -RGO and RuO 2 . This research may pave an effective way for photocatalytic hydrogen production utilizing solar light.
研究领域:
材料科学
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能源化学
·
纳米技术
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2019
·
IF 5.155
Wei Li,Qiong Ma,Xiao Wang,Shu-ao He,Min Li,Longfang Ren
Due to the increasing pressure of social environment and the increasing demand of human for energy, it is urgent to seek a sustainable and pollution-free new energy. Hydrogen is considered as a new type of energy because of its high calorific value , no environmental pollution and low cost of raw materials. In this experiment, to improve the visible-light driven catalytic activity of two-dimensional g-C 3 N 4 , g-C 3 N 4 and Ag/AgBr nanoparticles (NPs) were used as the carrier and cocatalyst, and the g-C 3 N 4 /Ag/AgBr (CNAA-α, α = 1, 2 and 3) heterojunction photocatalysts with different amounts of Ag/AgBr were synthesized via solvothermal technology. The morphology, composition , structure, photochemical and electrochemical characteristics of the samples were analyzed through XRD , FTIR , TEM , XPS and a series of photoelectrochemical characterizations, and the visible-light driven catalytic hydrogen evolution activities of the samples were studied by catalyzing water splitting. Research showed that the CNAA-2 exhibited the smallest overvoltage (86.5 mV vs RHE) and Tafel slope (61.0 mV·dec −1 ), so that the highest photocatalytic activity (47.84 μmol·g −1 ·h −1 ) for hydrogen evolution was obtained at the absence of Pt co-catalyst. Furthermore, this heterojunction photocatalyst exhibited good photostability and could be recycled several times with no significant decrease of its activity. This indicated that the addition of Ag/AgBr NPs to the two-dimensional g-C 3 N 4 nanosheets to construct an effective p-n heterojunction system at their interfaces could promote the conduction of photo-induced carriers and inhibit their combination, so that it would significantly improve the photoresponse ability and catalytic activity of two-dimensional g-C 3 N 4 nanosheets.
研究领域:
材料科学
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环境科学
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能源科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）