Nitrogen-doped carbon materials encapsulating 3 d transition metals are promising alternatives to replace noble metal Pt catalysts for efficiently catalyzing the oxygen reduction reaction(ORR). Herein, we use cobalt s...Nitrogen-doped carbon materials encapsulating 3 d transition metals are promising alternatives to replace noble metal Pt catalysts for efficiently catalyzing the oxygen reduction reaction(ORR). Herein, we use cobalt substituted perfluorosulfonic acid/polytetrafluoroethylene copolymer and dicyandiamide as the pyrolysis precursor to synthesize nitrogen-doped carbon nanotube(N–CNT) encapsulating cobalt nanoparticles hybrid material. The carbon layers and specific surface area of N–CNT have a critical role to the ORR performance due to the exposed active sites, determined by the mass ratio of the two precursors. The optimum hybrid material exhibits high ORR activity and stability, as well as excellent performance and durability in zinc–air battery.展开更多
The development of bifunctional oxygen electrocatalysts with high efficiency, high stability, and low cost is of great significance to the industrialization of rechargeable Zn–air batteries. A widely accepted view is...The development of bifunctional oxygen electrocatalysts with high efficiency, high stability, and low cost is of great significance to the industrialization of rechargeable Zn–air batteries. A widely accepted view is that the oxygen reduction reaction(ORR) and the oxygen evolution reaction(OER) follow different catalytic mechanisms, and accordingly they need different active sites for catalysis. Transition metal elements have admirable electronic acceptance ability for coordinating with reactants, and this can weaken the bond energy between reactants, thus promoting the ORR or OER reactions. Herein, the ORR and OER activities of different transition metal supported nitrogen-doped carbon nanotubes were systematically studied and compared. The optimal catalyst for synchronous ORR and OER was obtained by pyrolyzing melamine, cobalt nitrate, and nickel nitrate on carbon nanotubes, called cobalt–nickel supported nitrogenmixed carbon nanotubes(CoNi–NCNT), which were equipped with two types of high-performance active sites—the Co/Ni–N–C structure for the ORR and Co Ni alloy particles for the OER—simultaneously. Remarkably, the optimized Co Ni–NCNT exhibited a satisfactory bifunctional catalytic activity for both the ORR and OER. The value of the oxygen electrode activity parameter,△E, of CoNi–NCNT was 0.81 V, which surpasses that of catalysts Pt/C and Ir/C, and most of the non-precious metal-based bifunctional electrocatalysts reported in previous literatures. Furthermore, a specially assembled rechargeable Zn–air cell with Co Ni–NCNT loaded carbon paper as an air cathode was used to evaluate the practicability. As a result, a superior specific capacity of 744.3 mAh/gZn, a peak power density of 88 mW/cm2, and an excellent rechargeable cycling stability were observed, and these endow the Co Ni–NCNT with promising prospects for practical application.展开更多
The electro-Fenton process,with its capacity for in-situ H_(2)O_(2)formation and Fe^(2+)regeneration,is a strik-ing alternative to the traditional chemical-Fenton process.However,the frequent requirement of extra bind...The electro-Fenton process,with its capacity for in-situ H_(2)O_(2)formation and Fe^(2+)regeneration,is a strik-ing alternative to the traditional chemical-Fenton process.However,the frequent requirement of extra binders for electrode fabrication leads to low catalyst utilization,a complex fabrication process,and weak conductivity.Herein,a three-dimensional(3D)porous electrode was fabricated in-situ on a Ni foam(NF)substrate integrated with nitrogen-doped carbon nanotubes(N@C)derived from carbonization of zeolitic imidazolate framework-8(ZIF-8)without any binder.The resulting 900/N@C-NF cathode(synthesized at 900℃)was high in surface area,N content,and degree of graphitization,achieved high performance of H_(2)O_(2)production(2.58 mg L^(−1)h^(−1)H_(2)O_(2)/mg catalyst)at-0.7 V(vs.SCE),and enabled prompt regeneration of Fe^(2+).The electro-Fenton system equipped with the 900/N@C-NF cathode was effective in removing a diverse range of organic pollutants,including rhodamine B(Rh B),phenol,bisphenol A(BPA),nitroben-zene(NB),and Cu-ethylenediaminetetraacetic acid(EDTA),and significantly attenuating the concentration of chemical oxygen demand(COD)in the real acid wastewater,exhibiting superior activity and stability.This binder-free and self-supporting electro-Fenton cathode was thus shown to be an attractive candidate for application to wastewater treatment,particularly those rich in organics,acids,and Fe^(3+)/Fe^(2+).展开更多
基金financial support from the Ministry of Science and Technology of China(Grants 2016YFB0600901 and 2013CB933100)the National Natural Science Foundation of China(Grants 21573222 and 91545202)+1 种基金the Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDB17020200)financial support from CAS Youth Innovation Promotion(Grant No.2015145)
文摘Nitrogen-doped carbon materials encapsulating 3 d transition metals are promising alternatives to replace noble metal Pt catalysts for efficiently catalyzing the oxygen reduction reaction(ORR). Herein, we use cobalt substituted perfluorosulfonic acid/polytetrafluoroethylene copolymer and dicyandiamide as the pyrolysis precursor to synthesize nitrogen-doped carbon nanotube(N–CNT) encapsulating cobalt nanoparticles hybrid material. The carbon layers and specific surface area of N–CNT have a critical role to the ORR performance due to the exposed active sites, determined by the mass ratio of the two precursors. The optimum hybrid material exhibits high ORR activity and stability, as well as excellent performance and durability in zinc–air battery.
基金supported by the National Natural Science Foundation of China(21677171)。
文摘The development of bifunctional oxygen electrocatalysts with high efficiency, high stability, and low cost is of great significance to the industrialization of rechargeable Zn–air batteries. A widely accepted view is that the oxygen reduction reaction(ORR) and the oxygen evolution reaction(OER) follow different catalytic mechanisms, and accordingly they need different active sites for catalysis. Transition metal elements have admirable electronic acceptance ability for coordinating with reactants, and this can weaken the bond energy between reactants, thus promoting the ORR or OER reactions. Herein, the ORR and OER activities of different transition metal supported nitrogen-doped carbon nanotubes were systematically studied and compared. The optimal catalyst for synchronous ORR and OER was obtained by pyrolyzing melamine, cobalt nitrate, and nickel nitrate on carbon nanotubes, called cobalt–nickel supported nitrogenmixed carbon nanotubes(CoNi–NCNT), which were equipped with two types of high-performance active sites—the Co/Ni–N–C structure for the ORR and Co Ni alloy particles for the OER—simultaneously. Remarkably, the optimized Co Ni–NCNT exhibited a satisfactory bifunctional catalytic activity for both the ORR and OER. The value of the oxygen electrode activity parameter,△E, of CoNi–NCNT was 0.81 V, which surpasses that of catalysts Pt/C and Ir/C, and most of the non-precious metal-based bifunctional electrocatalysts reported in previous literatures. Furthermore, a specially assembled rechargeable Zn–air cell with Co Ni–NCNT loaded carbon paper as an air cathode was used to evaluate the practicability. As a result, a superior specific capacity of 744.3 mAh/gZn, a peak power density of 88 mW/cm2, and an excellent rechargeable cycling stability were observed, and these endow the Co Ni–NCNT with promising prospects for practical application.
基金supported by the National Natural Science Foundation of China (21106178)Postdoctoral Science Foundation of China (20110491480)+3 种基金Scientific Research Foundation of Xuzhou, China (XJ11B009)Polysilicon and Photovoltaic Energy Technology of Xuzhou, China (6AT102092)Open Fund of the State Key Laboratory of Advanced Technology for Materials Synthesis and Processing (Wuhan University of Technology) (2012-KF-13)Scientific Research Foundation for Yong Teachers of the China University of Mining and Technology, China (2011QNA21, 2009A026)~~
基金financial support from the Guangdong Special Support Plan for Innovation Teams (No.2019BT02L218)the Science and Technology Planning Project of Guangdong Province,China (No.2019A050510009)+3 种基金the Guangdong Special Support Plan for Young Top-notch Talents (No.2019TQ05L179)the National Natural Science Foundation of China (No.21876052)the Science and Technology Program of Guangzhou,China (No.201904010293)the Fundamental Research Funds for the Central Universities,SCUT (No.2020ZYGXZR055)。
文摘The electro-Fenton process,with its capacity for in-situ H_(2)O_(2)formation and Fe^(2+)regeneration,is a strik-ing alternative to the traditional chemical-Fenton process.However,the frequent requirement of extra binders for electrode fabrication leads to low catalyst utilization,a complex fabrication process,and weak conductivity.Herein,a three-dimensional(3D)porous electrode was fabricated in-situ on a Ni foam(NF)substrate integrated with nitrogen-doped carbon nanotubes(N@C)derived from carbonization of zeolitic imidazolate framework-8(ZIF-8)without any binder.The resulting 900/N@C-NF cathode(synthesized at 900℃)was high in surface area,N content,and degree of graphitization,achieved high performance of H_(2)O_(2)production(2.58 mg L^(−1)h^(−1)H_(2)O_(2)/mg catalyst)at-0.7 V(vs.SCE),and enabled prompt regeneration of Fe^(2+).The electro-Fenton system equipped with the 900/N@C-NF cathode was effective in removing a diverse range of organic pollutants,including rhodamine B(Rh B),phenol,bisphenol A(BPA),nitroben-zene(NB),and Cu-ethylenediaminetetraacetic acid(EDTA),and significantly attenuating the concentration of chemical oxygen demand(COD)in the real acid wastewater,exhibiting superior activity and stability.This binder-free and self-supporting electro-Fenton cathode was thus shown to be an attractive candidate for application to wastewater treatment,particularly those rich in organics,acids,and Fe^(3+)/Fe^(2+).
基金financially supported by the National Natural Science Foundation of China(21875062)State Key Laboratory of Pressure Hydrometallurgical Technology of Associated Nonferrous Metal Resources(yy20160012),China
基金supported by the National Natural Science Foundation of China(51872076 and U1804255)the Program for Innovative Research Team of Henan Scientific Committee(CXTD2014033)+1 种基金the Project of Central Plains Science and Technology Innovation Leading Talents of Henan Province(194200510001)the Scientific and Technological Research Project of Henan province(212102210651)。
