Traditional conversion of alcohols into carbonyl compounds exists a few drawbacks such as harsh reaction conditions,production of large amounts of hazardous wastes,and poor selectivity.The newly emerging conversion ap...Traditional conversion of alcohols into carbonyl compounds exists a few drawbacks such as harsh reaction conditions,production of large amounts of hazardous wastes,and poor selectivity.The newly emerging conversion approaches via photo-,electro-,and photoelectro-catalysis to oxidize alcohols into high value-added corresponding carbonyl compounds as well as the possible simultaneous production of clean fuel hydrogen(H_(2))under mild conditions are promising to substitute the traditional approach to form greener and sustainable reaction systems and thus have aroused tremendous investigations.In this review,the state-of-the-art photocatalytic,electrocatalytic,and photoelectrocatalytic strategies for selective oxidation of different types of alcohols(aromatic and aliphatic alcohols,single alcohol,and polyols,etc.)as well as the simultaneous production of H_(2) in certain systems are discussed.The design of photocatalysts,electrocatalysts,and photoelectrocatalysts as well as reaction mechanism is summarized and discussed in detail.In the end,current challenges and future research directions are proposed.It is expected that this review will not only deepen the understanding of environmentally friendly catalytic systems for alcohol conversion as well as H_(2) production,but also enlighten significance and inspirations for the follow-up study of selective oxidation of various types of organic molecules to value-added chemicals.展开更多
Synthesis of silver nanoparticles(Ag NPs) with state-of-the-art chemical or photo-reduction methods generally takes several steps and requires both reducing agents and stabilizers to obtain NPs with narrow size distri...Synthesis of silver nanoparticles(Ag NPs) with state-of-the-art chemical or photo-reduction methods generally takes several steps and requires both reducing agents and stabilizers to obtain NPs with narrow size distribution.Herein, we report a novel method to synthesize Ag NPs rapidly in one step, achieving typical particle sizes in the range from 5 to 15 nm.The synthesis steps only involve three chemicals without any reducing agent: AgNO3 as precursor, polyvinylpyrrolidone(PVP) as stabilizer, and AgCl as photocatalyst.The Ag NPs were supported on carbon and showed excellent performance in thermal catalytic pnitrophenol reduction and nitrobenzene hydrogenation, and as electrocatalyst for the oxygen reduction reaction.展开更多
In this work,a novel in situ auto-reduction strategy was developed to encapsulate uniformly dispersed Pd clusters/nanoparticles in MIL-125-NH_(2).It is demonstrated that the amino groups in MIL-125-NH_(2)can react wit...In this work,a novel in situ auto-reduction strategy was developed to encapsulate uniformly dispersed Pd clusters/nanoparticles in MIL-125-NH_(2).It is demonstrated that the amino groups in MIL-125-NH_(2)can react with formaldehyde to form novel reducing groups(-NH-CH_(2)OH),which can in situ auto-reduce the encapsulated Pd^(2+)ions to metallic Pd clusters/nanoparticles.As no additional reductants are required,the strategy limits the aggregation and migration of Pd clusters and the formation of large Pd nanoparticles via controlling the amount of Pd^(2+)precursor.When applied as catalysts in the hydrogenation of phenol in the aqueous phase,the obtained Pd(1.5)/MIL-125-NH-CH_(2)OH catalyst with highly dispersed Pd clusters/nanoparticles with the size of around 2 nm exhibited 100%of phenol conversion and 100%of cyclohexanone selectivity at 70℃ after 5 h,as well as remarkable reusability for at least five cycles due to the large MOF surface area,the highly dispersed Pd clusters/nanoparticles and their excellent stability within the MIL-125-NH-CH_(2)OH framework.展开更多
基金support from the National Natural Science Foundation of China(21976054,22176054)the Fundamental Research Funds for the Central Universities(2020MS036,FRF-TP-20-005A3)+1 种基金the Fundamental Research Funds for the Central Universities and the Youth Teacher International Exchange&Growth Program(QNXM20220026)MOE Key Laboratory of Resources and Environmental System Optimization,College of Environmental Science and Engineering,North China Electric Power University(KLRE-KF202201)。
文摘Traditional conversion of alcohols into carbonyl compounds exists a few drawbacks such as harsh reaction conditions,production of large amounts of hazardous wastes,and poor selectivity.The newly emerging conversion approaches via photo-,electro-,and photoelectro-catalysis to oxidize alcohols into high value-added corresponding carbonyl compounds as well as the possible simultaneous production of clean fuel hydrogen(H_(2))under mild conditions are promising to substitute the traditional approach to form greener and sustainable reaction systems and thus have aroused tremendous investigations.In this review,the state-of-the-art photocatalytic,electrocatalytic,and photoelectrocatalytic strategies for selective oxidation of different types of alcohols(aromatic and aliphatic alcohols,single alcohol,and polyols,etc.)as well as the simultaneous production of H_(2) in certain systems are discussed.The design of photocatalysts,electrocatalysts,and photoelectrocatalysts as well as reaction mechanism is summarized and discussed in detail.In the end,current challenges and future research directions are proposed.It is expected that this review will not only deepen the understanding of environmentally friendly catalytic systems for alcohol conversion as well as H_(2) production,but also enlighten significance and inspirations for the follow-up study of selective oxidation of various types of organic molecules to value-added chemicals.
基金the financial support from the National Natural Science Foundation of China (61574065)Science and Technology Planning Project of Guangdong Province (2016B090906004, 2016B090918083)+7 种基金the Special Fund Project of Science and Technology Application in Guangdong (2017B020240002)graduate student abroad joint training project of South China Normal Universitypartially supported by PCSIRT Project No.IRT_17R40Guangdong Provincial Key Laboratory of Optical Information Materials and Technology (No.2017B030301007)MOE International Laboratory for Optical Information TechnologiesShenzhen Science and Technology Plan (No.JSGG20170414143009027)National 111 ProjectGuangdong Innovative Research Team Program (No.2013C102)
文摘Synthesis of silver nanoparticles(Ag NPs) with state-of-the-art chemical or photo-reduction methods generally takes several steps and requires both reducing agents and stabilizers to obtain NPs with narrow size distribution.Herein, we report a novel method to synthesize Ag NPs rapidly in one step, achieving typical particle sizes in the range from 5 to 15 nm.The synthesis steps only involve three chemicals without any reducing agent: AgNO3 as precursor, polyvinylpyrrolidone(PVP) as stabilizer, and AgCl as photocatalyst.The Ag NPs were supported on carbon and showed excellent performance in thermal catalytic pnitrophenol reduction and nitrobenzene hydrogenation, and as electrocatalyst for the oxygen reduction reaction.
基金financial support from the National Natural Science Foundation of China(Grant No.51802015)the Research Department Closed Carbon Cycle Economy(CCCE)at the Ruhr-University Bochum,Fundamental Research Funds for the Central Universities(No.FRF-TP-20-005A3)the Fundamental Research Funds for the Central Universities and the Youth Teacher International Exchange&Growth Program(Grant No.QNXM20210016)。
文摘In this work,a novel in situ auto-reduction strategy was developed to encapsulate uniformly dispersed Pd clusters/nanoparticles in MIL-125-NH_(2).It is demonstrated that the amino groups in MIL-125-NH_(2)can react with formaldehyde to form novel reducing groups(-NH-CH_(2)OH),which can in situ auto-reduce the encapsulated Pd^(2+)ions to metallic Pd clusters/nanoparticles.As no additional reductants are required,the strategy limits the aggregation and migration of Pd clusters and the formation of large Pd nanoparticles via controlling the amount of Pd^(2+)precursor.When applied as catalysts in the hydrogenation of phenol in the aqueous phase,the obtained Pd(1.5)/MIL-125-NH-CH_(2)OH catalyst with highly dispersed Pd clusters/nanoparticles with the size of around 2 nm exhibited 100%of phenol conversion and 100%of cyclohexanone selectivity at 70℃ after 5 h,as well as remarkable reusability for at least five cycles due to the large MOF surface area,the highly dispersed Pd clusters/nanoparticles and their excellent stability within the MIL-125-NH-CH_(2)OH framework.