Ammonia serves as a crucial chemical raw material and hydrogen energy carrier.Aqueous electrocatalytic nitrogen reduction reaction(NRR),powered by renewable energy,has attracted tremendous interest during the past few...Ammonia serves as a crucial chemical raw material and hydrogen energy carrier.Aqueous electrocatalytic nitrogen reduction reaction(NRR),powered by renewable energy,has attracted tremendous interest during the past few years.Although some achievements have been revealed in aqueous NRR,significant challenges have also been identified.The activity and selectivity are fundamentally limited by nitrogen activation and competitive hydrogen evolution.This review focuses on the hurdles of nitrogen activation and delves into complementary strategies,including materials design and system optimization(reactor,electrolyte,and mediator).Then,it introduces advanced interdisciplinary technologies that have recently emerged for nitrogen activation using high-energy physics such as plasma and triboelectrification.With a better understanding of the corresponding reaction mechanisms in the coming years,these technologies have the potential to be extended in further applications.This review provides further insight into the reaction mechanisms of selectivity and stability of different reaction systems.We then recommend a rigorous and detailed protocol for investigating NRR performance and also highlight several potential research directions in this exciting field,coupling with advanced interdisciplinary applications,in situ/operando characterizations,and theoretical calculations.展开更多
Ammonia is a commodity chemical with high added value.Electrochemical reduction of nitrogen has great promise for the sustainable synthesis of ammonia in recent vears.Because of its rich resources and unique electroni...Ammonia is a commodity chemical with high added value.Electrochemical reduction of nitrogen has great promise for the sustainable synthesis of ammonia in recent vears.Because of its rich resources and unique electronic structure and characteristics,2D transition metal compounds have been used as electrocatalysts for electro-chemical reduction of nitrogen for clean and sustainable production of ammonia,This review outlines the latest development in the use of 2D transition metal compounds as high-efficiency electrocatalysts for nitrogen reduction.reaction(NRR).First,we introduce the N,reduction mechanism,and briefly summarize the performance indicators ofthe catalyst.Then,we focused on the functionalization of unique 2D materials to design high-performance 2D electrocatalysts in respect of simulation calculation and experimental development.Finally,the current challenges and future opportunities for NRR electrocatalvsts are introduced.展开更多
Electrochemical nitrogen reduction reaction(NRR) to produce ammonia under ambient conditions is considered as a promising approach to tackle the energy-intensive Haber-Bosch process,but the low Faradaic efficiency and...Electrochemical nitrogen reduction reaction(NRR) to produce ammonia under ambient conditions is considered as a promising approach to tackle the energy-intensive Haber-Bosch process,but the low Faradaic efficiency and yield of NH_3 are still a challenge.Herein,a carbon-vacancies enriched mesoporous g-C_3 N_4 is developed by an in situ Zr doping strategy.The in situ mesoporous-forming mechanism is deeply understood by TPSR to reveal the functions of Zr dopant that pulls C from the precursor of C_3 N_4,resulting the formation of homogeneous mesopores with about 57% of the one C-defective s-triazine ring in C_3 N_4.Due to the defect sites obtained in metal doping synthesis,the RuAu bimetallic supported catalyst(RuAu_3/0.3 Zr-C_3 N_4) exhibits effective NRR performance with a Faraday efficiency of 11.54% and an NH_3 yield of 5.28 μg h^(-1) mg_(cat) ^(-1).at-0.1 V(RHE),which is nearly 10 times higher than that of RuAu_3/C_3 N_4 catalyst.This work proposes a simple and template-free preparation method for the high defect density mesoporous C_3 N_4,and provides new possibilities of a wide application of mesopore g-C3 N4.展开更多
基金Natural Sciences and Engineering Research Council of Canada (NSERC)Fonds de Recherche du Québec-Nature et Technologies (FRQNT)+3 种基金Centre Québécois sur les Materiaux Fonctionnels (CQMF)Institut National de la Recherche Scientifique (INRS)École de Technologie Supérieure (ÉTS)King Abdullah University of Science and Technology (KAUST)。
文摘Ammonia serves as a crucial chemical raw material and hydrogen energy carrier.Aqueous electrocatalytic nitrogen reduction reaction(NRR),powered by renewable energy,has attracted tremendous interest during the past few years.Although some achievements have been revealed in aqueous NRR,significant challenges have also been identified.The activity and selectivity are fundamentally limited by nitrogen activation and competitive hydrogen evolution.This review focuses on the hurdles of nitrogen activation and delves into complementary strategies,including materials design and system optimization(reactor,electrolyte,and mediator).Then,it introduces advanced interdisciplinary technologies that have recently emerged for nitrogen activation using high-energy physics such as plasma and triboelectrification.With a better understanding of the corresponding reaction mechanisms in the coming years,these technologies have the potential to be extended in further applications.This review provides further insight into the reaction mechanisms of selectivity and stability of different reaction systems.We then recommend a rigorous and detailed protocol for investigating NRR performance and also highlight several potential research directions in this exciting field,coupling with advanced interdisciplinary applications,in situ/operando characterizations,and theoretical calculations.
基金Supported by the Natural Science Foundation of Ningxia,China(No.2018AAC03012)the National Natural Science Foundation of China(No.21765016)+1 种基金the Ningxia Leading Scientific and Technological Innovation Talents Project.China(No.KJT2018002)the National First-rate Discipline Project of Ningxia,China(NXYLXK2017404)。
文摘Ammonia is a commodity chemical with high added value.Electrochemical reduction of nitrogen has great promise for the sustainable synthesis of ammonia in recent vears.Because of its rich resources and unique electronic structure and characteristics,2D transition metal compounds have been used as electrocatalysts for electro-chemical reduction of nitrogen for clean and sustainable production of ammonia,This review outlines the latest development in the use of 2D transition metal compounds as high-efficiency electrocatalysts for nitrogen reduction.reaction(NRR).First,we introduce the N,reduction mechanism,and briefly summarize the performance indicators ofthe catalyst.Then,we focused on the functionalization of unique 2D materials to design high-performance 2D electrocatalysts in respect of simulation calculation and experimental development.Finally,the current challenges and future opportunities for NRR electrocatalvsts are introduced.
基金supported by the National Natural Science Foundation of China (No. 21978259)the Zhejiang Provincial Natural Science Foundation of China (No. LR17B060002)the Fundamental Research Funds for the Central Universities。
文摘Electrochemical nitrogen reduction reaction(NRR) to produce ammonia under ambient conditions is considered as a promising approach to tackle the energy-intensive Haber-Bosch process,but the low Faradaic efficiency and yield of NH_3 are still a challenge.Herein,a carbon-vacancies enriched mesoporous g-C_3 N_4 is developed by an in situ Zr doping strategy.The in situ mesoporous-forming mechanism is deeply understood by TPSR to reveal the functions of Zr dopant that pulls C from the precursor of C_3 N_4,resulting the formation of homogeneous mesopores with about 57% of the one C-defective s-triazine ring in C_3 N_4.Due to the defect sites obtained in metal doping synthesis,the RuAu bimetallic supported catalyst(RuAu_3/0.3 Zr-C_3 N_4) exhibits effective NRR performance with a Faraday efficiency of 11.54% and an NH_3 yield of 5.28 μg h^(-1) mg_(cat) ^(-1).at-0.1 V(RHE),which is nearly 10 times higher than that of RuAu_3/C_3 N_4 catalyst.This work proposes a simple and template-free preparation method for the high defect density mesoporous C_3 N_4,and provides new possibilities of a wide application of mesopore g-C3 N4.
