利用可再生能源驱动的电催化C-N偶联来合成尿素可以取代高能耗、高污染的工业生产尿素过程.然而,同时提高尿素收率和相应的法拉第效率,目前仍面临挑战.在此,我们设计了富氧空位的Ru掺杂CeO_(2)电催化剂用于高效电化学合成尿素.通过调节R...利用可再生能源驱动的电催化C-N偶联来合成尿素可以取代高能耗、高污染的工业生产尿素过程.然而,同时提高尿素收率和相应的法拉第效率,目前仍面临挑战.在此,我们设计了富氧空位的Ru掺杂CeO_(2)电催化剂用于高效电化学合成尿素.通过调节Ru的比例,发现最佳掺杂量为5%,该Ru-CeO_(2)电催化剂在电压为-0.7 V vs.RHE时能提供20.2 mmol h^(-1)g^(-1)的高尿素产率和20.1%法拉第效率,优于大多数已报道的催化剂.实验结果表明,Ru掺杂和氧空位的协同效应优化了反应物的吸附和活化,增强了C-N偶联的动力学,并显著提高了电化学合成尿素的效率.本工作将为开发高效合成尿素的先进C-N偶联电催化剂提供借鉴.展开更多
Solar-driven H_(2)O_(2)production and emerging organic pollutants(EOPs)elimination are of great significance from the perspective of environmental sustainability.The efficiency of the photocatalytic reaction system is...Solar-driven H_(2)O_(2)production and emerging organic pollutants(EOPs)elimination are of great significance from the perspective of environmental sustainability.The efficiency of the photocatalytic reaction system is the key challenge to be addressed.In this work,the strategy of constructing surface ionic local polarization centers to enhance the exciton dissociation of the polymeric photocatalytic is demonstrated.Selected bipyridinium cation(TMAP)is complexed on a K^(+)-incorporated carbon nitride(CNK)framework,and the combination of local polarization centers both on the surface(bipyridinium cation)and bulk(K+cation)contributes to a superior photocatalytic H_(2)O_(2)production performance,affording a remarkable H_(2)O_(2)generation rate of 46.8μmol h^(-1)mg^(-1)and a high apparent quantum yield(AQY)value of 77.5%under irradiation of 405 nm photons.As substantiated experimentally by steady state/transient spectroscopy techniques,the surface local polarization centers increase the population of the long-lived trapped electrons,and thereby promote the interfacial charge transfer process for chemical conversion reaction.The strategy is potentially applicable to the design of a wide range of efficient solar-to-chemical conversion systems.展开更多
基金supported by the Key Projects of Intergovernmental International Cooperation in Key R&D Programs of the Ministry of Science and Technology of China(2021YFE0115800)the National Science Funding Committee of China(U20A20250)。
文摘利用可再生能源驱动的电催化C-N偶联来合成尿素可以取代高能耗、高污染的工业生产尿素过程.然而,同时提高尿素收率和相应的法拉第效率,目前仍面临挑战.在此,我们设计了富氧空位的Ru掺杂CeO_(2)电催化剂用于高效电化学合成尿素.通过调节Ru的比例,发现最佳掺杂量为5%,该Ru-CeO_(2)电催化剂在电压为-0.7 V vs.RHE时能提供20.2 mmol h^(-1)g^(-1)的高尿素产率和20.1%法拉第效率,优于大多数已报道的催化剂.实验结果表明,Ru掺杂和氧空位的协同效应优化了反应物的吸附和活化,增强了C-N偶联的动力学,并显著提高了电化学合成尿素的效率.本工作将为开发高效合成尿素的先进C-N偶联电催化剂提供借鉴.
基金Financial supports by the National Natural Science Foundation of China(No.21976041)Guangzhou Municipal Science and Technology Project(No.202201020168)+1 种基金Tertiary Education Scientific Research Project of Guangzhou Municipal Education Bureau(No.202235238)Guangdong Basic and Applied Basic Research Foundation(No.2023A1515010788)are acknowledged。
文摘Solar-driven H_(2)O_(2)production and emerging organic pollutants(EOPs)elimination are of great significance from the perspective of environmental sustainability.The efficiency of the photocatalytic reaction system is the key challenge to be addressed.In this work,the strategy of constructing surface ionic local polarization centers to enhance the exciton dissociation of the polymeric photocatalytic is demonstrated.Selected bipyridinium cation(TMAP)is complexed on a K^(+)-incorporated carbon nitride(CNK)framework,and the combination of local polarization centers both on the surface(bipyridinium cation)and bulk(K+cation)contributes to a superior photocatalytic H_(2)O_(2)production performance,affording a remarkable H_(2)O_(2)generation rate of 46.8μmol h^(-1)mg^(-1)and a high apparent quantum yield(AQY)value of 77.5%under irradiation of 405 nm photons.As substantiated experimentally by steady state/transient spectroscopy techniques,the surface local polarization centers increase the population of the long-lived trapped electrons,and thereby promote the interfacial charge transfer process for chemical conversion reaction.The strategy is potentially applicable to the design of a wide range of efficient solar-to-chemical conversion systems.
