The existing industrial ammonia synthesis usually adopts the Haber-Bosch process,which requires harsh conditions of high temperature and high pressure,and consumes high energy.Under this circumstance,photoelectrochemi...The existing industrial ammonia synthesis usually adopts the Haber-Bosch process,which requires harsh conditions of high temperature and high pressure,and consumes high energy.Under this circumstance,photoelectrochemical(PEC)catalysis is regarded as a promising method for N_(2) reduction reaction(NRR),but bears problems of low efficiency and yield.Thus,exploring active catalysts remains highly desirable.In this work,BiVO_(4)@MXene hybrids have been facilely synthesized by a hydrothermal route.The heterojunctions by the in situ growth of BiVO_(4) onto two-dimensional(2D)MXene greatly increase the NRR efficiency:under photoelectric conditions,the optimized NH_(3) yield is 27.25µg h^(-1) cm^(-2),and the Faraday efficiency achieves 17.54% at−0.8 V relative to the reversible hydrogen electrode(RHE),which are higher than most state-of-the-art NRR(photo)electrocatalysts.The mechanism speculation shows the enhanced light absorption range and the heterojunction formation largely promote the separation and the transfer efficiency of photogenerated carriers,thereby improving the PEC catalytic ability.Therefore,this work provides a hybrid route to combine the advantages of photo and electric catalysis for effective artificial nitrogen fixation.展开更多
基金supported by the National Natural Science Foundation of China(Nos.21771021,21822501,21725303,22061130206 and 22120102005)the Beijing Municipal Natural Science Fundation(No.JQ20003)+3 种基金the Newton Advanced Fellowship award(No.NAFR1201285)the Fok Ying-Tong Education Foundation(No.171008)the Measurements Fund of Beijing Normal Universitythe State Key Laboratory of Heavy Oil Processing.
文摘The existing industrial ammonia synthesis usually adopts the Haber-Bosch process,which requires harsh conditions of high temperature and high pressure,and consumes high energy.Under this circumstance,photoelectrochemical(PEC)catalysis is regarded as a promising method for N_(2) reduction reaction(NRR),but bears problems of low efficiency and yield.Thus,exploring active catalysts remains highly desirable.In this work,BiVO_(4)@MXene hybrids have been facilely synthesized by a hydrothermal route.The heterojunctions by the in situ growth of BiVO_(4) onto two-dimensional(2D)MXene greatly increase the NRR efficiency:under photoelectric conditions,the optimized NH_(3) yield is 27.25µg h^(-1) cm^(-2),and the Faraday efficiency achieves 17.54% at−0.8 V relative to the reversible hydrogen electrode(RHE),which are higher than most state-of-the-art NRR(photo)electrocatalysts.The mechanism speculation shows the enhanced light absorption range and the heterojunction formation largely promote the separation and the transfer efficiency of photogenerated carriers,thereby improving the PEC catalytic ability.Therefore,this work provides a hybrid route to combine the advantages of photo and electric catalysis for effective artificial nitrogen fixation.
