Total conversion of centimeter -scale nickel foam into single atom electrocatalysts with highly selective CO, electrocatalytic reduction in neutral electrolyte

被引:28
作者
Fan, Qikui [1 ,2 ]
Gao, Pengfei [3 ]
Ren, Shan [4 ]
Qu, Yunteng [5 ]
Kong, Chuncai [1 ]
Yang, Jian [2 ]
Wu, Yuen [6 ]
机构
[1] Xi An Jiao Tong Univ, Sch Phys, Shaanxi Prov Key Lab Adv Funct Mat & Mesoscop Phy, Minist Educ,Key Lab Nonequilibrium Synth & Modula, Xian 710049, Peoples R China
[2] Shenzhen Univ, Coll Mat Sci & Engn, Guangdong Res Ctr Interfacial Engn Funct Mat, Shenzhen Key Lab Special Funct Mat, Shenzhen 518060, Peoples R China
[3] Northwest Inst Nucl Technol, Xian 710024, Peoples R China
[4] Soothow Univ, Inst Funct Nano & Soft Mat FUNSOM, Jiangsu Key Lab Carbon Based Funct Mat & Devices, Suzhou 215123, Peoples R China
[5] Northwest Univ, Inst Photon & Photon Technol, Int Collaborat Ctr Photoelect Technol & Nano Func, State Key Lab Photoelect Technol & Funct Mat, Xian 710069, Peoples R China
[6] Univ Sci & Technol China, IChEM Collaborat Innovat Ctr Chem Energy Mat, Dept Chem, Hefei 230026, Peoples R China
基金
中国国家自然科学基金;
关键词
Ni single atom electrocatalyst; CO2 electroreduction to CO; neutral electrolyte; thermal diffusion; CARBON-DIOXIDE; ELECTROREDUCTION; CATALYSTS; METAL; SITES;
D O I
10.1007/s12274-022-4472-6
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
To improve the atomic utilization of metals and reduce the cost of industrialization, the one-step total monoatomization of macroscopic bulk metals, as opposed to nanoscale metals, is effective. In this study, we used a thermal diffusion method to directly convert commercial centimeter-scale Ni foam to porous Ni single -atom -loaded carbon nanotubes (CNT5). As expected, owing to the coating of single -atom on porous, highly conductive CNT carriers, Ni single-atom electrocatalysts (Ni-SACs) exhibit extremely high activity and selectivity in CO2 electroreduction (CO2RR), yielding a current density of > 350 mNcm(2), a selectivity for CO of > 91% under a flow cell configuration using a 1 M potassium chloride (KCI) electrolyte. Based on the superior activity of the Ni-SACs electrocatalyst, an integrated gas -phase electrochemical zero-gap reactor was introduced to generate a significant amount of CO current for potential practical applications. The overall current can be increased to 800 mA, while maintaining CO Faradaic efficiencies (FEs) at above 90% per unit cell. Our findings and insights on the active site transformation mechanism for macroscopic bulk Ni foam conversion into single atoms can inform the design of highly active single -atom catalysts used in industrial CO2RR systems.
引用
收藏
页码:2003 / 2010
页数:8
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