Elucidating the activity, mechanism and application of selective electrosynthesis of ammonia from nitrate on cobalt phosphide

Shenghua Ye; Zhida Chen; Guikai Zhang; Wenda Chen; Chao Peng; Xiuyuan Yang; Lirong Zheng; Yongliang Li; Xiangzhong Ren; Huiqun Cao; Dongfeng Xue; Jieshan Qiu; Qianling Zhang; Jianhong Liu

doi:10.1039/D1EE03097C

Elucidating the activity, mechanism and application of selective electrosynthesis of ammonia from nitrate on cobalt phosphide†

Shenghua Ye,‡^ab Zhida Chen,‡^a Guikai Zhang,^c Wenda Chen,^a Chao Peng,^d Xiuyuan Yang,^d Lirong Zheng,

*^c Yongliang Li,

^a Xiangzhong Ren,^a Huiqun Cao,^a Dongfeng Xue,

*^d Jieshan Qiu,*^e Qianling Zhang

*^a and Jianhong Liu*^ab

Author affiliations

* Corresponding authors

^a Graphene Composite Research Center, College of Chemistry and Environmental Engineering, Shenzhen University, Shenzhen 518060, P. R. China
E-mail: zhql@szu.edu.cn, liujh@szu.edu.cn

^b Shenzhen Eigen-Equation Graphene Technology Co. Ltd., Shenzhen 518000, P. R. China

^c Institute of High Energy Physics Chinese Academy of Sciences, Beijing 100049, P. R. China
E-mail: zhenglr@ihep.ac.cn

^d Multiscale Crystal Materials Research Center, Shenzhen Institute of Advanced Technology, Chinese Academy of Sciences, Shenzhen 518055, China
E-mail: df.xue@siat.ac.cn

^e College of Chemical Engineering, Beijing University of Chemical Technology, Beijing, China
E-mail: qiujs@mail.buct.edu.cn

Abstract

Electrochemical reduction of nitrate to ammonia (nitrate reduction reaction, NO₃⁻RR) under ambient conditions, which overcomes the drawbacks of the energy-intensive Haber–Bosch reaction and low-efficient N₂ electroreduction, is one of the alternatives toward ammonia-synthesis. In this study, cobalt phosphide nanosheet arrays (CoP NAs) grown on carbon fiber cloth (CFC) (CoP NAs/CFC) exhibit an ammonia-evolving rate of 9.56 mol h⁻¹ m⁻² (214.14 L h⁻¹ m⁻², STP) at −0.3 V vs. RHE with a Faraday efficiency of ∼100% under alkaline conditions, which goes far beyond the Haber–Bosch reaction. Phosphorus was proved to be crucial for stabilizing the active phase and optimizing the energy barriers of the NO₃⁻RR. Moreover, operando X-ray absorption fine structure (XAFS) firstly revealed that Co 4p orbitals directly participate in the nitrate adsorption and electron transfer step of the NO₃⁻RR. Eventually, combining the NO₃⁻RR and benzyl alcohol oxidation reaction at the cathode and anode respectively, sustainable synthesis of value-added chemicals was successfully fulfilled.

Energy & Environmental Science

Elucidating the activity, mechanism and application of selective electrosynthesis of ammonia from nitrate on cobalt phosphide†

Abstract

Supplementary files

Article information

Download Citation

Permissions

Elucidating the activity, mechanism and application of selective electrosynthesis of ammonia from nitrate on cobalt phosphide

Social activity

Search articles by author

Spotlight

Advertisements