The photo-induced vapor-phase decomposition of dimethyl ether was investigated on Pt metals deposited on pure and N-doped TiO2. Infrared spectroscopic measurements revealed that adsorption of dimethyl ether on TiO2 sa...The photo-induced vapor-phase decomposition of dimethyl ether was investigated on Pt metals deposited on pure and N-doped TiO2. Infrared spectroscopic measurements revealed that adsorption of dimethyl ether on TiO2 samples underwent partial dissociation to methoxy species. Illumination of the (CH3)2O-TiO2 and (CH3)2O-M/TiO2 systems led to the conversion of methoxy into adsorbed formate. In the case of metal-promoted TiO2 catalysts, CO bonded to the metals was also detected. Pure titania exhibited a very little photoactivity. Deposition of Pt metals on TiO2 markedly enhanced the extent of photocatalytic decomposition of dimethyl ether to give H2 and CO2 as the major products. A small amount of CO and methyl formate was also identified in the products. The most active metal was the Rh followed by Pd, Ir, Pt and Ru. When the bandgap of TiO2 was lowered by N-doping, the photocatalytic activity of metal/TiO2 catalysts appreciably increased. The effect of metals was explained by a better separation of charge carriers induced by illumination and by enhanced electronic interaction between metal nanoparticles and TiO2.展开更多
Photocatalytic and photoelectrochemical water splitting using semiconductor materials are effective approaches for converting solar energy into hydrogen fuel.In the past few years,a series of photocatalysts/photoelect...Photocatalytic and photoelectrochemical water splitting using semiconductor materials are effective approaches for converting solar energy into hydrogen fuel.In the past few years,a series of photocatalysts/photoelectrocatalysts have been developed and optimized to achieve efficient solar hydrogen production.Among various optimization strategies,the regulation of spin polarization can tailor the intrinsic optoelectronic properties for retarding charge recombination and enhancing surface reactions,thus improving the solar-to-hydrogen(STH)efficiency.This review presents recent advances in the regulation of spin polarization to enhance spin polarized-dependent solar hydrogen evolution activity.Specifically,spin polarization manipulation strategies of several typical photocatalysts/photoelectrocatalysts(e.g.,metallic oxides,metallic sulfides,non-metallic semiconductors,ferroelectric materials,and chiral molecules)are described.In the end,the critical challenges and perspectives of spin polarization regulation towards future solar energy conversion are briefly provided.展开更多
Metal-organic frameworks(MOFs) with high designability and structure diversity have been widely developed as promising photocatalytic materials,but most of them suffer from poor charge transportation and separation ef...Metal-organic frameworks(MOFs) with high designability and structure diversity have been widely developed as promising photocatalytic materials,but most of them suffer from poor charge transportation and separation efficiency.To address it,the construction of MOFs-based heterostructures has been thus highly inspired.In this minireview,we will first introduce the basic principles of photocata lytic water splitting and heterostructure systems,and then discuss state-of-the-art MOFs-based heterostructures for photocata lytic water splitting to produce hydrogen.Meanwhile,special attention will be paid to the key factors affecting the interfacial charge transfer of heterostructures,such as interface connection mode,morphology control,and modification.Eventually,the challenges and prospects faced by the construction of high-efficiency MOFs-based heterostructure water slitting photocatalysts are proposed.展开更多
Suffering from the inefficient traditional trial-and-error methods and the huge searching space filled by millions of candidates, discovering new perovskite visible photocatalysts with higher hydrogen production rate(...Suffering from the inefficient traditional trial-and-error methods and the huge searching space filled by millions of candidates, discovering new perovskite visible photocatalysts with higher hydrogen production rate(RH_(2)) still remains a challenge in the field of photocatalytic water splitting(PWS). Herein, we established structural-property models targeted to RH_(2) and the proper bandgap(Eg) via machine learning(ML) technology to accelerate the discovery of efficient perovskite photocatalysts for PWS. The Pearson correlation coefficients(R) of leave-one-out cross validation(LOOCV) were adopted to compare the performances of different algorithms including gradient boosting regression(GBR), support vector regression(SVR), backpropagation artificial neural network(BPANN), and random forest(RF). It was found that the BPANN model showed the highest R values from LOOCV and testing data of 0.9897 and 0.9740 for RH_(2),while the GBR model had the best values of 0.9290 and 0.9207 for Eg. Furtherly, 14 potential PWS perovskite candidates were screened out from 30,000 ABO3-type perovskite structures under the criteria of structural stability, Eg, conduction band energy, valence band energy and RH_(2). The average RH_(2) of these14 perovskites is 6.4% higher than the highest value in the training data set. Moreover, the online web servers were developed to share our prediction models, which could be accessible in http://materialsdata-mining.com/ocpmdm/material_api/ahfga3d9puqlknig(E_g prediction) and http://materials-datamining.com/ocpmdm/material_api/i0 ucuyn3 wsd14940(RH_(2) prediction).展开更多
Two Cu-Mo-Fe-Ox samples, which can store and supply pure hydrogen through repeated redox reaction （Fe3O4＋4H23Fe＋4H2O）, were prepared by co-precipitation （FCM-C） and impregnation （FCM-I） methods, respectively, ...Two Cu-Mo-Fe-Ox samples, which can store and supply pure hydrogen through repeated redox reaction （Fe3O4＋4H23Fe＋4H2O）, were prepared by co-precipitation （FCM-C） and impregnation （FCM-I） methods, respectively, and the performance of hydrogen production from water were investigated. Compared with the impregnated sample, the co-precipitation sample presented better catalytic activity. The samples were characterized by X-ray diffraction （XRD）, field emission scanning electron microscopy （FE-SEM）, X-ray photoelectron spectroscopy （XPS）, Fourier transform infrared spectroscopy （FT-IR） and temperature-programmed reduction （H2-TPR） techniques. XRD, FE-SEM and XPS results suggest that the FCM-C sample has smaller particle size and higher dispersion of iron oxide than that of FCM-I sample. In addition, FT-IR and H2-TPR analyses indicate that the weak interaction among metal oxides in FCM-C sample may induce facile reduction of active metal and superior property of hydrogen production by decomposing water in success展开更多
Hydrogen peroxide has attracted increasing interest as an environmentally benign and green oxidant that can also be used as a solar fuel in fuel cells.This review focuses on recent progress in production of hydrogen p...Hydrogen peroxide has attracted increasing interest as an environmentally benign and green oxidant that can also be used as a solar fuel in fuel cells.This review focuses on recent progress in production of hydrogen peroxide by solar-light-driven oxidation of water by dioxygen and its usage as a green oxidant and fuel.The photocatalytic production of hydrogen peroxide is made possible by combining the e^(-)and 4e-oxidation of water with the e^(-)reduction of dioxygen using solar energy.The catalytic control of the selectivity of the e^(-)vs.4e-oxidation of water is discussed together with the selectivity of the e^(-)vs.4e-reduction of dioxygen.The combination of the photocatalytic e^(-)oxidation of water and the e^(-)reduction of dioxygen provides the best efficiency because both processes afford hydrogen peroxide.The solar-light-driven hydrogen peroxide production by oxidation of water and by reduction of dioxygen is combined with the catalytic oxidation of substrates with hydrogen peroxides,in which dioxygen is used as the greenest oxidant.展开更多
Integrating the hydrogen production technologies from renewable energy with the advanced distributed hydrogen power systems has being become an important development trend of energy science and technology in the twent...Integrating the hydrogen production technologies from renewable energy with the advanced distributed hydrogen power systems has being become an important development trend of energy science and technology in the twenty-first century, since it may satisfactorily solve such problems met in the utilization of renewable energy as low density, instability, discontinuity and changing with time, season and climate. In this paper, the status and prospect of studies on hydrogen production theories and technologies from renewable energy especially the photocatalytic water splitting and the thermochemical catalytic gasification of biomass in supercritical water are commented on, and some new suggestions to build up novel hydrogen energy power system based on renewable energy are put forward.展开更多
文摘The photo-induced vapor-phase decomposition of dimethyl ether was investigated on Pt metals deposited on pure and N-doped TiO2. Infrared spectroscopic measurements revealed that adsorption of dimethyl ether on TiO2 samples underwent partial dissociation to methoxy species. Illumination of the (CH3)2O-TiO2 and (CH3)2O-M/TiO2 systems led to the conversion of methoxy into adsorbed formate. In the case of metal-promoted TiO2 catalysts, CO bonded to the metals was also detected. Pure titania exhibited a very little photoactivity. Deposition of Pt metals on TiO2 markedly enhanced the extent of photocatalytic decomposition of dimethyl ether to give H2 and CO2 as the major products. A small amount of CO and methyl formate was also identified in the products. The most active metal was the Rh followed by Pd, Ir, Pt and Ru. When the bandgap of TiO2 was lowered by N-doping, the photocatalytic activity of metal/TiO2 catalysts appreciably increased. The effect of metals was explained by a better separation of charge carriers induced by illumination and by enhanced electronic interaction between metal nanoparticles and TiO2.
基金support from the National Natural Science Foundation of China(No.22105031)National Key Research and Development Program of China(No.2019YFE0121600)+2 种基金Sichuan Science and Technology Program(No.2021YFH0054,2023JDGD0011)Fundamental Research Funds for the Central Universities(ZYGX2020J028)Z.M.W.acknowledges the National Key Research and Development Program of China(No.2019YFB2203400)and the“111 Project”(No.B20030).
文摘Photocatalytic and photoelectrochemical water splitting using semiconductor materials are effective approaches for converting solar energy into hydrogen fuel.In the past few years,a series of photocatalysts/photoelectrocatalysts have been developed and optimized to achieve efficient solar hydrogen production.Among various optimization strategies,the regulation of spin polarization can tailor the intrinsic optoelectronic properties for retarding charge recombination and enhancing surface reactions,thus improving the solar-to-hydrogen(STH)efficiency.This review presents recent advances in the regulation of spin polarization to enhance spin polarized-dependent solar hydrogen evolution activity.Specifically,spin polarization manipulation strategies of several typical photocatalysts/photoelectrocatalysts(e.g.,metallic oxides,metallic sulfides,non-metallic semiconductors,ferroelectric materials,and chiral molecules)are described.In the end,the critical challenges and perspectives of spin polarization regulation towards future solar energy conversion are briefly provided.
基金supported by the National Natural Science Foundation of China(21633009,21925206,21901240)the Dalian National Laboratory for Clean Energy(DNL)Cooperation Fund,CAS(no.DNL 201913)+3 种基金DICP&QIBEBT(UN201805)International Partnership Program of Chinese Academy of Sciences(121421KYSB20190025)the DICP foundation of innovative research(DICP I201927)the support from Liao Ning Revitalization Talents Program(XLYC1807241)。
文摘Metal-organic frameworks(MOFs) with high designability and structure diversity have been widely developed as promising photocatalytic materials,but most of them suffer from poor charge transportation and separation efficiency.To address it,the construction of MOFs-based heterostructures has been thus highly inspired.In this minireview,we will first introduce the basic principles of photocata lytic water splitting and heterostructure systems,and then discuss state-of-the-art MOFs-based heterostructures for photocata lytic water splitting to produce hydrogen.Meanwhile,special attention will be paid to the key factors affecting the interfacial charge transfer of heterostructures,such as interface connection mode,morphology control,and modification.Eventually,the challenges and prospects faced by the construction of high-efficiency MOFs-based heterostructure water slitting photocatalysts are proposed.
基金Financial support to this work from the National Key Research and Development Program of China (No. 2016YFB0700504)the Science and Technology Commission of Shanghai Municipality (18520723500) is gratefully acknowledged。
文摘Suffering from the inefficient traditional trial-and-error methods and the huge searching space filled by millions of candidates, discovering new perovskite visible photocatalysts with higher hydrogen production rate(RH_(2)) still remains a challenge in the field of photocatalytic water splitting(PWS). Herein, we established structural-property models targeted to RH_(2) and the proper bandgap(Eg) via machine learning(ML) technology to accelerate the discovery of efficient perovskite photocatalysts for PWS. The Pearson correlation coefficients(R) of leave-one-out cross validation(LOOCV) were adopted to compare the performances of different algorithms including gradient boosting regression(GBR), support vector regression(SVR), backpropagation artificial neural network(BPANN), and random forest(RF). It was found that the BPANN model showed the highest R values from LOOCV and testing data of 0.9897 and 0.9740 for RH_(2),while the GBR model had the best values of 0.9290 and 0.9207 for Eg. Furtherly, 14 potential PWS perovskite candidates were screened out from 30,000 ABO3-type perovskite structures under the criteria of structural stability, Eg, conduction band energy, valence band energy and RH_(2). The average RH_(2) of these14 perovskites is 6.4% higher than the highest value in the training data set. Moreover, the online web servers were developed to share our prediction models, which could be accessible in http://materialsdata-mining.com/ocpmdm/material_api/ahfga3d9puqlknig(E_g prediction) and http://materials-datamining.com/ocpmdm/material_api/i0 ucuyn3 wsd14940(RH_(2) prediction).
基金supported by the National Basic Research Program of China(973 Program,2011CB201202)of Ministry of Science and Technology of China(MOST)
文摘Two Cu-Mo-Fe-Ox samples, which can store and supply pure hydrogen through repeated redox reaction （Fe3O4＋4H23Fe＋4H2O）, were prepared by co-precipitation （FCM-C） and impregnation （FCM-I） methods, respectively, and the performance of hydrogen production from water were investigated. Compared with the impregnated sample, the co-precipitation sample presented better catalytic activity. The samples were characterized by X-ray diffraction （XRD）, field emission scanning electron microscopy （FE-SEM）, X-ray photoelectron spectroscopy （XPS）, Fourier transform infrared spectroscopy （FT-IR） and temperature-programmed reduction （H2-TPR） techniques. XRD, FE-SEM and XPS results suggest that the FCM-C sample has smaller particle size and higher dispersion of iron oxide than that of FCM-I sample. In addition, FT-IR and H2-TPR analyses indicate that the weak interaction among metal oxides in FCM-C sample may induce facile reduction of active metal and superior property of hydrogen production by decomposing water in success
基金supported by the JSPS KAKENHI(16H02268)from MEXTJapan and by the CRI(2012R1A3A2048842)Basic Science Research Program(NRF-2020R1I1A1A01074630)through NRF of Korea.
文摘Hydrogen peroxide has attracted increasing interest as an environmentally benign and green oxidant that can also be used as a solar fuel in fuel cells.This review focuses on recent progress in production of hydrogen peroxide by solar-light-driven oxidation of water by dioxygen and its usage as a green oxidant and fuel.The photocatalytic production of hydrogen peroxide is made possible by combining the e^(-)and 4e-oxidation of water with the e^(-)reduction of dioxygen using solar energy.The catalytic control of the selectivity of the e^(-)vs.4e-oxidation of water is discussed together with the selectivity of the e^(-)vs.4e-reduction of dioxygen.The combination of the photocatalytic e^(-)oxidation of water and the e^(-)reduction of dioxygen provides the best efficiency because both processes afford hydrogen peroxide.The solar-light-driven hydrogen peroxide production by oxidation of water and by reduction of dioxygen is combined with the catalytic oxidation of substrates with hydrogen peroxides,in which dioxygen is used as the greenest oxidant.
基金This work is supported by NSFC project and the national science foundation for outstanding young scientists, and the Special Funds for Major State Basic Research Projects of China.
文摘Integrating the hydrogen production technologies from renewable energy with the advanced distributed hydrogen power systems has being become an important development trend of energy science and technology in the twenty-first century, since it may satisfactorily solve such problems met in the utilization of renewable energy as low density, instability, discontinuity and changing with time, season and climate. In this paper, the status and prospect of studies on hydrogen production theories and technologies from renewable energy especially the photocatalytic water splitting and the thermochemical catalytic gasification of biomass in supercritical water are commented on, and some new suggestions to build up novel hydrogen energy power system based on renewable energy are put forward.
