Electrocatalytic Reduction of Nitrate to Ammonia on Low-Cost Ultrathin CoOxNanosheets

Wang，Jing1,2; Cai，Chao3; Wang，Yian2; Yang，Xuming1; Wu，Duojie1; Zhu，Yuanmin1; Li，Menghao1; Gu，Meng1; Shao，Minhua2,4

2021

10.1021/acscatal.1c03918

ACS Catalysis   影响因子和分区

2155-5435

2155-5435

The electrochemical nitrate reduction reaction (NITRR) is an appealing method for ammonia synthesis, owing to the ambient conditions as well as its abundant sources, low dissociation energy, and high solubility of nitrate. The hydrogen evolution reaction is a competing process of the NITRR, which should be properly suppressed to achieve a high Faradaic efficiency of the NITRR. Herein, ultrathin CoOx nanosheets with abundant surface oxygen are designed as a low-cost NITRR catalyst, which delivers an ultrahigh ammonia yield of 82.4 ± 4.8 mg h-1 mgcat-1 with a Faradaic efficiency of 93.4 ± 3.8% at -0.3 V versus the reversible hydrogen electrode. Theoretical calculation reveals that the surface oxygen on cobalt sites can stabilize the adsorbed hydrogen on cobalt oxide, which hampers the evolution of hydrogen and leads to an enhanced NITRR activity. This work demonstrates that surface modification plays a critical role in suppressing the HER and facilitating the NITRR through a NHO pathway with a lower energy barrier.

ammonia cobalt oxide electrocatalysis nitrate reduction reaction surface oxygen

SCI ; EI

英语

ESI热点 ; ESI高被引

第一 ; 通讯

Shenzhen National Natural Science Foundation of China[21802065] ; Shenzhen Science and Technology Program[KQTD20190929173815000] ; Shenzhen Natural Science Fund[20200925154115001] ; Guangdong Innovative and Entrepreneurial Research Team Program[2019ZT08C044] ; Innovation and Technology Commission of the Hong Kong Special Administrative Region[ITC-CNERC14EG03] ; Hunan Provincial Science and Technology Program[2020RC2004]

Chemistry

Chemistry, Physical

WOS:000751835200044

AMER CHEMICAL SOC

20215011330207

Cobalt compounds ; Costs ; Electrocatalysis ; Nitrates ; Reduction ; Surface reactions

Electrochemistry:801.4.1 ; Chemical Reactions:802.2 ; Inorganic Compounds:804.2 ; Cost and Value Engineering; Industrial Economics:911

2-s2.0-85121036378

Scopus

1.Department of Materials Science and Engineering,Southern University of Science and Technology,Shenzhen,Guangdong,518055,China
2.Department of Chemical and Biological Engineering,Hong Kong University of Science and Technology,Kowloon,Clear Water Bay,Hong Kong
3.School of Physics and Electronics,Central South University,Changsha,Hunan,410083,China
4.Energy Institute,Chinese National Engineering Research Center for Control and Treatment of Heavy Metal Pollution,Hong Kong University of Science and Technology,Kowloon,Clear Water Bay,Hong Kong

Wang，Jing,Cai，Chao,Wang，Yian,et al. Electrocatalytic Reduction of Nitrate to Ammonia on Low-Cost Ultrathin CoOxNanosheets[J]. ACS Catalysis,2021,11(24):15135-15140.

Wang，Jing.,Cai，Chao.,Wang，Yian.,Yang，Xuming.,Wu，Duojie.,...&Shao，Minhua.(2021).Electrocatalytic Reduction of Nitrate to Ammonia on Low-Cost Ultrathin CoOxNanosheets.ACS Catalysis,11(24),15135-15140.

Wang，Jing,et al."Electrocatalytic Reduction of Nitrate to Ammonia on Low-Cost Ultrathin CoOxNanosheets".ACS Catalysis 11.24(2021):15135-15140.