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1.
Sustainable hydrogen production is attracting increasing attention and visible-light-driven water splitting is considered as one of the most promising approaches for hydrogen evolution and solar energy storage. Different materials have been screened at mild conditions in recent decades and 2-dimensional (2D) layered materials are considered good candidates for the photocatalytic water splitting reaction. 2D single layer MoS2 has shown its potential in various catalytic systems, and has also been used in photocatalytic water splitting reaction recently. However, current studies of MoS2 monolayers give low intrinsic activity, preventing it from practical applications. This is attributed to the rapid recombination of the photo-excited charge carriers at room temperature, resulting in poor quantum efficiency (QE). Herein, a state-of-the-art strategy to prolong the exciton lifetimes is reported, which is achieved by combining the 2D MoS2 nanosheets with solid state polar-faceted supports. The charge separation process can be facilitated by the strong local polarisation introduced by the polar-faceted supports, and tuned by changing the supports with different surface polarities. Polar oxide surface is the exposure of oxygen-terminated high energetic facet, which is known to give a net dipole moment perpendicular to its surface. Such variation in the surface properties of the support to the above metal would lead to a difference in metal-support interaction(s). The resulting composite structures show great enhancement toward the visible-light-driven photocatalytic water splitting reaction, giving hydrogen and oxygen evolution in a stoichiometric 2:1 ratio at elevated temperatures from pure water. Photocatalytic performances are improved by the prolonged exciton lifetimes and exceptional hydrogen evolution activity of 2977 μmol g−1 h−1 with impressive QEs are obtained over Ru-doped MoS2 nanosheets on polar ceria support, which is among the best of the reported results of similar catalytic systems to date. More excitingly, the linear relationship between the exciton lifetimes and strength of the local polarisation is also observed, indicating that the rational design of photocatalysts can be simply achieved via engineering their local polarisation by incorporation of polar-faceted materials. 相似文献
2.
利用可见光催化分解水制氢的研究进展 总被引:1,自引:0,他引:1
简述了利用可见光催化分解水制氢的基本原理及该领域的最新研究进展.由能带模型概述了设计可见光响应催化剂的3种方案,重点介绍了元素掺杂类型光催化剂、氮氧/硫氧化物光催化剂、固溶体催化剂等可见光催化分解水体系.阐述了该课题的重要意义及面临的巨大挑战,提出了未来该领域需要加强研究的若干问题. 相似文献
3.
Lei Wang Yangyang Wan Yanjun Ding Sikai Wu Ying Zhang Xinlei Zhang Guoqing Zhang Yujie Xiong Xiaojun Wu Jinlong Yang Hangxun Xu 《Advanced materials (Deerfield Beach, Fla.)》2017,29(38)
Direct water splitting into H2 and O2 using photocatalysts by harnessing sunlight is very appealing to produce storable chemical fuels. Conjugated polymers, which have tunable molecular structures and optoelectronic properties, are promising alternatives to inorganic semiconductors for water splitting. Unfortunately, conjugated polymers that are able to efficiently split pure water under visible light (400 nm) via a four‐electron pathway have not been previously reported. This study demonstrates that 1,3‐diyne‐linked conjugated microporous polymer nanosheets (CMPNs) prepared by oxidative coupling of terminal alkynes such as 1,3,5‐tris‐(4‐ethynylphenyl)‐benzene (TEPB) and 1,3,5‐triethynylbenzene (TEB) can act as highly efficient photocatalysts for splitting pure water (pH ≈ 7) into stoichiometric amounts of H2 and O2 under visible light. The apparent quantum efficiencies at 420 nm are 10.3% and 7.6% for CMPNs synthesized from TEPB and TEB, respectively; the measured solar‐to‐hydrogen conversion efficiency using the full solar spectrum can reach 0.6%, surpassing photosynthetic plants in converting solar energy to biomass (globally average ≈0.10%). First‐principles calculations reveal that photocatalytic H2 and O2 evolution reactions are energetically feasible for CMPNs under visible light irradiation. The findings suggest that organic polymers hold great potential for stable and scalable solar‐fuel generation. 相似文献
4.
Hsieh SH Lee GJ Chen CY Chen JH Ma SH Horng TL Chen KH Wu JJ 《Journal of nanoscience and nanotechnology》2012,12(7):5930-5936
This study was focused on the preparation of modified bismuth oxide photocatalysts, including Ru and Pt doped Bi2O3, using sonochemically assisted method to enhance their photocatalytic activity. The crystalline phase composition and surface structure of Bi2O3 photocatalysts were examined using SEM, XRD, UV-visible spectroscopy, and XPS. Optical characterizations have indicated that the Bi2O3 presents the photoabsorption properties shifting from UV light region into visible light which is approaching towards the edge of 470 nm. According to the experimental results, visible-light-driven photocatalysis for water splitting with the addition of 0.3 M Na2SO3 and 0.03 M H2C2O4 as sacrificing agents demonstrates that Pt/Bi2O3-RuO2 catalyst could increase the amount of hydrogen evolution, which is around 11.6 and 14.5 micromol g(-1) h(-1), respectively. Plausible formation mechanisms of modified bismuth oxide and reaction mechanisms of photocatalytic water splitting have been proposed. 相似文献
5.
Xinlei Zhang Xiao Luo Xusheng Zheng Xiaojun Wu Hangxun Xu 《Small (Weinheim an der Bergstrasse, Germany)》2019,15(43)
Ultrathin 2D conjugated polymer nanosheets are an emerging class of photocatalysts for solar‐to‐chemical energy conversion. Until now, the majority of ultrathin 2D polymer photocatalysts are produced through exfoliation of layered polymers. Unfortunately, it still remains a great challenge to exfoliate layered polymers into ultrathin nanosheets with high yields. In this work, a liquid‐phase protonation‐assisted exfoliation is demonstrated to enable remarkably improved exfoliation yields of various 2D N‐containing conjugated polymers such as g‐C3N4, C2N, and aza‐CMP. The exfoliation yields are only 2–15% in pure water whereas they can be substantially improved to 41–56% in 12 m HCl. The exfoliated ultrathin nanosheets possess average thicknesses less than 5 nm and can be easily dispersed in aqueous solutions. More importantly, the exfoliated nanosheets exhibit significantly enhanced photocatalytic activity toward photocatalytic water splitting compared to their bulk counterparts. Further characterizations and computational calculations reveal that protonation of the heterocyclic nitrogen sites in the conjugated polymer frameworks can lead to strong hydrogen bonding between the polymer surfaces and water molecules, resulting in facilitated exfoliation of polymers into the liquid phase. This study unveils an important protocol toward producing ultrathin 2D N‐containing conjugated polymer nanosheets for future solar energy conversion. 相似文献
6.
Photocatalytic water splitting into hydrogen and oxygen is a method to directly convert light energy into storable chemical energy, and has received considerable attention for use in large-scale solar energy utilization. Particulate semiconductors are generally used as photocatalysts, and semiconductor properties such as bandgap, band positions, and photocarrier mobility can heavily impact photocatalytic performance. The design of active photocatalysts has been performed with the consideration of such semiconductor properties. Photocatalysts have a catalytic aspect in addition to a semiconductor one. The ability to control surface redox reactions in order to efficiently produce targeted reactants is also important for photocatalysts. Over the past few decades, various photocatalysts for water splitting have been developed, and a recent main concern has been the development of visible-light sensitive photocatalysts for water splitting. This review introduces the study of water-splitting photocatalysts, with a focus on recent progress in visible-light induced overall water splitting on oxynitride photocatalysts. Various strategies for designing efficient photocatalysts for water splitting are also discussed herein. 相似文献
7.
Xiangchen Kong Huiming Huang Zhaoyang Li Yanqin Liang Zhenguo Li Shengli Zhu 《材料科学技术学报》2021,80(21):171-178
TiO2 (B) nanosheets/GO (graphene oxide) hybrids are considered to be outstanding performance pho-tocatalysts for high efficiency of H2 evolution.However,they still suffer severe challenges during the synthetic processes,such as a large amount of the capping agents adhering on the surface and easy occurrence of aggregation.To figure out these obstacles,Ar plasma treatment as a modified method in this study not only enable the TiO2 (B) nanosheets distributed uniformly on the GO sheets but also engi-neer defects within TiO2 (B) nanosheetsto significantly improve the photocatalytic activity for the water splitting.The hydrogen evolution rate of the TiO2-x (B)/GO sheets is 1.4 times higher compared with that of original TiO2 (B)/GO sheets without Ar plasma treatment.The improved photocatalytic proper-ties were owing to the synergetic effects of oxygen vacancies and the heterojunction between GO and TiO2 (B),which can promote the visible light utilization and accelerate separation and transportation of photogenerated electron-holes.This study can provide a facile pathway to prepare the two-dimensional hybrid photocatalysts with high photocatalytic H2 activity. 相似文献
8.
AbstractPhotocatalytic water splitting into hydrogen and oxygen is a method to directly convert light energy into storable chemical energy, and has received considerable attention for use in large-scale solar energy utilization. Particulate semiconductors are generally used as photocatalysts, and semiconductor properties such as bandgap, band positions, and photocarrier mobility can heavily impact photocatalytic performance. The design of active photocatalysts has been performed with the consideration of such semiconductor properties. Photocatalysts have a catalytic aspect in addition to a semiconductor one. The ability to control surface redox reactions in order to efficiently produce targeted reactants is also important for photocatalysts. Over the past few decades, various photocatalysts for water splitting have been developed, and a recent main concern has been the development of visible-light sensitive photocatalysts for water splitting. This review introduces the study of water-splitting photocatalysts, with a focus on recent progress in visible-light induced overall water splitting on oxynitride photocatalysts. Various strategies for designing efficient photocatalysts for water splitting are also discussed herein. 相似文献
9.
Yuval Ben‐Shahar Francesco Scotognella Nir Waiskopf Ilka Kriegel Stefano Dal Conte Giulio Cerullo Uri Banin 《Small (Weinheim an der Bergstrasse, Germany)》2015,11(4):462-471
Hybrid semiconductor–metal nanoparticles are interesting materials for use as photocatalysts due to their tunable properties and chemical processibility. Their function in the evolution of hydrogen in photocatalytic water splitting is the subject of intense current investigation. Here, the effects of the surface coatings on the photocatalytic function are studied, with Au‐tipped CdS nanorods as a model hybrid nanoparticle system. Kinetic measurements of the hydrogen evolution rate following photocatalytic water reduction are performed on similar nanoparticles but with different surface coatings, including various types of thiolated alkyl ligands and different polymer coatings. The apparent hydrogen evolution quantum yields are found to strongly depend on the surface coating. The lowest yields are observed for thiolated alkyl ligands. Intermediate values are obtained with L‐glutathione and poly(styrene‐co‐maleic anhydride) polymer coatings. The highest efficiency is obtained for polyethylenimine (PEI) polymer coating. These pronounced differences in the photocatalytic efficiencies are correlated with ultrafast transient absorption spectroscopy measurements, which show a faster bleach recovery for the PEI‐coated hybrid nanoparticles, consistent with faster and more efficient charge separation. These differences are primarily attributed to the effects of surface passivation by the different coatings affecting the surface trapping of charge carriers that compete with effective charge separation required for the photocatalysis. Further support of this assignment is provided from steady‐state emission and time‐resolved spectral measurements, performed on related strongly fluorescing CdSe/CdS nanorods. The control and understanding of the effect of the surface coating of the hybrid nanosystems on the photocatalytic processes is of importance for the potential application of hybrid nanoparticles as photocatalysts. 相似文献
10.
Motonori Watanabe 《Science and Technology of Advanced Materials》2013,14(1):705-723
AbstractRenewable hydrogen production is a sustainable method for the development of next-generation energy technologies. Utilising solar energy and photocatalysts to split water is an ideal method to produce hydrogen. In this review, the fundamental principles and recent progress of hydrogen production by artificial photosynthesis are reviewed, focusing on hydrogen production from photocatalytic water splitting using organic–inorganic composite-based photocatalysts. 相似文献
11.
《Advanced Powder Technology》2020,31(1):11-28
Harvesting solar energy attracts great attention due to its abundant, clean, and permanent characteristics. Thus, photocatalysts have emerged as promising candidates for converting the solar energy to practically useful hydrogen molecules. Tremendous efforts have been devoted in developments of efficient photocatalysts for water splitting, but most of photocatalysts utilize noble metals to improve photocatalytic performance. Progress in photocatalyst materials for the hydrogen production coupled with a better understanding of the basic catalytic mechanisms has enabled better selection of catalytic nanomaterials with improved performance. In this review, we analyze the current state of the art in photocatalyst materials for photochemical hydrogen production through water splitting using earth-abundant materials. We also explore two main factors involved in both material morphology and sacrificial agent to further improve the activity, efficiency and stability of photocatalysts. 相似文献
12.
Wei-Cheng Lin Chih-Li Chang Chin-Hsuan Shih Wan-Chi Lin Ze- Yu Lai Je-Wei Chang Li-Yu Ting Tse-Fu Huang Yu-En Sun Hung-Yi Huang Yu-Tung Lin Jia-Jen Liu Yi-Hsiang Wu Yuan-Ting Tseng Ying-Rang Zhuang Bing-Heng Li An-Chung Su Chi-Hua Yu Chin-Wen Chen Kun-Han Lin U-Ser Jeng Ho-Hsiu Chou 《Small (Weinheim an der Bergstrasse, Germany)》2023,19(42):2302682
Conjugated polymers (CPs) have recently gained increasing attention as photocatalysts for sunlight-driven hydrogen evolution. However, they suffer from insufficient electron output sites and poor solubility in organic solvents, severely limiting their photocatalytic performance and applicability. Herein, solution-processable all–acceptor (A1–A2)-type CPs based on sulfide-oxidized ladder-type heteroarene are synthesized. A1–A2-type CPs showed upsurging efficiency improvements by two to three orders of magnitude, compared to their donor–acceptor -type CP counterparts. Furthermore, by seawater splitting, PBDTTTSOS exhibited an apparent quantum yield of 18.9% to 14.8% at 500 to 550 nm. More importantly, PBDTTTSOS achieved an excellent hydrogen evolution rate of 35.7 mmol h−1 g−1 and 150.7 mmol h−1 m−2 in the thin-film state, which is among the highest efficiencies in thin film polymer photocatalysts to date. This work provides a novel strategy for designing polymer photocatalysts with high efficiency and broad applicability. 相似文献
13.
Recent Progress in Cobalt‐Based Heterogeneous Catalysts for Electrochemical Water Splitting 下载免费PDF全文
Jiahai Wang Wei Cui Qian Liu Zhicai Xing Abdullah M. Asiri Xuping Sun 《Advanced materials (Deerfield Beach, Fla.)》2016,28(2):215-230
Water electrolysis is considered as the most promising technology for hydrogen production. Much research has been devoted to developing efficient electrocatalysts for hydrogen production via the hydrogen evolution reaction (HER) and oxygen production via the oxygen evolution reaction (OER). The optimum electrocatalysts can drive down the energy costs needed for water splitting via lowering the overpotential. A number of cobalt (Co)‐based materials have been developed over past years as non‐noble‐metal heterogeneous electrocatalysts for HER and OER. Recent progress in this field is summarized here, especially highlighting several important bifunctional catalysts. Various approaches to improve or optimize the electrocatalysts are introduced. Finally, the current existing challenges and the future working directions for enhancing the performance of Co‐implicated electrocatalysts are proposed. 相似文献
14.
15.
《工程(英文)》2017,3(3):365-378
Photocatalytic water splitting, which directly converts solar energy into hydrogen, is one of the most desirable solar-energy-conversion approaches. The ultimate target of photocatalysis is to explore efficient and stable photocatalysts for solar water splitting. Tantalum (oxy)nitride-based materials are a class of the most promising photocatalysts for solar water splitting because of their narrow bandgaps and sufficient band energy potentials for water splitting. Tantalum (oxy)nitride-based photocatalysts have experienced intensive exploration, and encouraging progress has been achieved over the past years. However, the solar-to-hydrogen (STH) conversion efficiency is still very far from its theoretical value. The question of how to better design these materials in order to further improve their water-splitting capability is of interest and importance. This review summarizes the development of tantalum (oxy)nitride-based photocatalysts for solar water spitting. Special interest is paid to important strategies for improving photocatalytic water-splitting efficiency. This paper also proposes future trends to explore in the research area of tantalum-based narrow bandgap photocatalysts for solar water splitting. 相似文献
16.
Nano-Micro Letters - As BiVO4 is one of the most popular visible-light-responding photocatalysts, it has been widely used for visible-light-driven water splitting and environmental purification.... 相似文献
17.
Chao-Peng Wang Yu-Xuan Lin Lei Cui Jian Zhu Xian-He Bu 《Small (Weinheim an der Bergstrasse, Germany)》2023,19(15):2207342
Hydrogen, a clean and flexible energy carrier, can be efficiently produced by electrocatalytic water splitting. To accelerate the sluggish hydrogen evolution reaction and oxygen evolution reaction kinetics in the splitting process, highly active electrocatalysts are essential for lowering the energy barriers, thereby improving the efficiency of overall water splitting. Combining the distinctive advantages of metal–organic frameworks (MOFs) with the physicochemical properties of 2D materials such as large surface area, tunable structure, accessible active sites, and enhanced conductivity, 2D MOFs have attracted intensive attention in the field of electrocatalysis. Different strategies, such as improving the conductivities of MOFs, reducing the thicknesses of MOF nanosheets, and integrating MOFs with conductive particles or substrates, are developed to promote the catalytic performances of pristine MOFs. This review summarizes the recent advances of pristine 2D MOF-based electrocatalysts for water electrolysis. In particular, their intrinsic electrocatalytic properties are detailly analyzed to reveal important roles of inherent MOF active centers, or other in situ generated active phases from MOFs responsible for the catalytic reactions. Finally, the challenges and development prospects of pristine 2D MOFs for the future applications in overall water splitting are discussed. 相似文献
18.
《工程(英文)》2021,7(7):991-1001
Semiconductor photocatalysis is a potential pathway to solve the problems of global energy shortage and environmental pollution. Black phosphorus (BP) has been widely used in the field of photocatalysis owing to its features of high hole mobility, adjustable bandgap, and wide optical absorption range. Nevertheless, pristine BP still exhibits unsatisfactory photocatalytic activity due to the low separation efficiency of photoinduced charge carriers. In recent years, the construction of heterostructured photocatalysts based on BP has become a research hotspot in photocatalysis with the remarkable improvement of photoexcited charge-separation efficiency. Herein, progress on the design, synthesis, properties, and applications of BP and its corresponding heterostructured photocatalysts is summarized. Furthermore, the photocatalytic applications of BP-based heterostructured photocatalysts in water splitting, pollutant degradation, carbon dioxide reduction, nitrogen fixation, bacterial disinfection, and organic synthesis are reviewed. Opportunities and challenges for the exploration of advanced BP-based heterostructured photocatalysts are presented. This review will promote the development and applications of BP-based heterostructured photocatalysts in energy conversion and environmental remediation. 相似文献
19.
Ultrathin 2D Photocatalysts: Electronic‐Structure Tailoring,Hybridization, and Applications 下载免费PDF全文
As a sustainable technology, semiconductor photocatalysis has attracted considerable interest in the past several decades owing to the potential to relieve or resolve energy and environmental‐pollution issues. By virtue of their unique structural and electronic properties, emerging ultrathin 2D materials with appropriate band structure show enormous potential to achieve efficient photocatalytic performance. Here, the state‐of‐the‐art progress on ultrathin 2D photocatalysts is reviewed and a critical appraisal of the classification, controllable synthesis, and formation mechanism of ultrathin 2D photocatalysts is presented. Then, different strategies to tailor the electronic structure of ultrathin 2D photocatalysts are summarized, including component tuning, thickness tuning, doping, and defect engineering. Hybridization with the introduction of a foreign component and maintaining the ultrathin 2D structure is presented to further boost the photocatalytic performance, such as quantum dots/2D materials, single atoms/2D materials, molecular/2D materials, and 2D–2D stacking materials. More importantly, the advancement of versatile photocatalytic applications of ultrathin 2D photocatalysts in the fields of water oxidation, hydrogen evolution, CO2 reduction, nitrogen fixation, organic syntheses, and removal pollutants is discussed. Finally, the future opportunities and challenges regarding ultrathin 2D photocatalysts to bring about new opportunities for future research in the field of photocatalysis are also presented. 相似文献
20.
《材料科学技术学报》2020,(3)
The ease of molecular design and functionalization make organic semiconductors(OSCs) unit the electronic, chemical and mechanical benefits with a material structure. The easily tunable optoelectronic properties of OSCs also make it promising building blocks and thereby provide more possibilities in photocatalytic applications. So far, organic nanostructures have gained great impetus and found wide applications in photocatalytic organic synthesis, remediation of water and air, as well as water splitting into hydrogen. But they still suffer from low charge separation and sunlight absorption efficiencies.Accordingly, many strategies have been explored to address these issues, and one of the most effective solutions is to develop nano-heterostructures. To give an impulse for the developments of this field, this review attempts to make a systematic introduction on the recent progress over the rational design and fabrication of organic nano-heterostructured photocatalysts, including the types of organic semiconductor/semiconductor(OSC/SC), organic semiconductor/metal(OSC/M), organic semiconductor/carbon(OSC/C), and OSC-based multinary nano-heterostructures. The emphasis is placed on the structure/property relationships, and their photocatalytic purposes in environmental and energy fields.At last, future challenges and perspectives for the ongoing development of OSC materials and their use in high-quality optoelectronic devices are also covered. 相似文献