Efficient electrocatalytic nitrogen reduction to ammonia with aqueous silver nanodots
Li, Wenyi1,2; Li, Ke1; Ye, Yixing1; Zhang, Shengbo1; Liu, Yanyan1,2; Wang, Guozhong1; Liang, Changhao1; Zhang, Haimin1; Zhao, Huijun3
刊名COMMUNICATIONS CHEMISTRY
2021-12-29
卷号4
ISSN号2399-3669
DOI10.1038/s42004-021-00449-7
通讯作者Liang, Changhao(chliang@issp.ac.cn) ; Zhang, Haimin(zhanghm@issp.ac.cn)
英文摘要The electrocatalytic nitrogen (N-2) reduction reaction (NRR) relies on the development of highly efficient electrocatalysts and electrocatalysis systems. Herein, we report a non-loading electrocatalysis system, where the electrocatalysts are dispersed in aqueous solution rather than loading them on electrode substrates. The system consists of aqueous Ag nanodots (AgNDs) as the catalyst and metallic titanium (Ti) mesh as the current collector for electrocatalytic NRR. The as-synthesized AgNDs, homogeneously dispersed in 0.1 M Na2SO4 solution (pH = 10.5), can achieve an NH3 yield rate of 600.4 +/- 23.0 mu g h(-1) mg(Ag)(-1) with a faradaic efficiency (FE) of 10.1 +/- 0.7% at -0.25 V (vs. RHE). The FE can be further improved to be 20.1 +/- 0.9% at the same potential by using Ti mesh modified with oxygen vacancy-rich TiO2 nanosheets as the current collector. Utilizing the aqueous AgNDs catalyst, a Ti plate based two-electrode configured flow-type electrochemical reactor was developed to achieve an NH3 yield rate of 804.5 +/- 30.6 mu g h(-1) mg(Ag)(-1) with a FE of 8.2 +/- 0.5% at a voltage of -1.8 V. The designed non-loading electrocatalysis system takes full advantage of the AgNDs' active sites for N-2 adsorption and activation, following an alternative hydrogenation mechanism revealed by theoretical calculations.
资助项目Natural Science Foundation of China[51872292] ; Natural Science Foundation of China[51571186] ; CAS/SAFEA International Partnership Program for Creative Research Teams of Chinese Academy of Sciences, China
WOS关键词HYDROGEN-EVOLUTION REACTION ; TOTAL-ENERGY CALCULATIONS ; N-2 REDUCTION ; QUANTUM DOTS ; CATALYSTS ; DIOXIDE ; DESIGN ; ELECTROREDUCTION ; NANOSHEETS ; FIXATION
WOS研究方向Chemistry
语种英语
出版者NATURE RESEARCH
WOS记录号WOS:000613476600001
资助机构Natural Science Foundation of China ; CAS/SAFEA International Partnership Program for Creative Research Teams of Chinese Academy of Sciences, China
内容类型期刊论文
源URL[http://ir.hfcas.ac.cn:8080/handle/334002/119683]  
专题中国科学院合肥物质科学研究院
通讯作者Liang, Changhao; Zhang, Haimin
作者单位1.Chinese Acad Sci, Anhui Key Lab Nanomat & Nanotechnol, CAS Ctr Excellence Nanosci,Inst Solid State Phys, HFIPS,Key Lab Mat Phys,Ctr Environm & Energy Nano, Hefei 230031, Peoples R China
2.Univ Sci & Technol China, Hefei 230026, Peoples R China
3.Griffith Univ, Ctr Clean Environm & Energy, Gold Coast Campus, Griffith, Qld, Australia
推荐引用方式
GB/T 7714
Li, Wenyi,Li, Ke,Ye, Yixing,et al. Efficient electrocatalytic nitrogen reduction to ammonia with aqueous silver nanodots[J]. COMMUNICATIONS CHEMISTRY,2021,4.
APA Li, Wenyi.,Li, Ke.,Ye, Yixing.,Zhang, Shengbo.,Liu, Yanyan.,...&Zhao, Huijun.(2021).Efficient electrocatalytic nitrogen reduction to ammonia with aqueous silver nanodots.COMMUNICATIONS CHEMISTRY,4.
MLA Li, Wenyi,et al."Efficient electrocatalytic nitrogen reduction to ammonia with aqueous silver nanodots".COMMUNICATIONS CHEMISTRY 4(2021).
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