Regulating Ni site in NiV LDH for efficient electrocatalytic production of formate and hydrogen by glycerol electrolysis  

作　　者：Lin Dong Guan-Ru Chang Yi Feng Xian-Zhi Yao Xin-Yao Yu 

机构地区：[1]Key Laboratory of Structure and Functional Regulation of Hybrid Materials,Institutes of Physical Science and Information Technology,Anhui University,Ministry of Education.Hefei 230601,China [2]School of Chemistry and Chemical Engineering,Huangshan University,Huangshan 245041,China [3]Department of Polymer Materials and Engineering,Academy of Chemical Engineering,Hebei University of Technology,Tianjin 300130,China [4]Ningbo Research Institute of Ecological and Environmental Sciences,Ningbo 315000,China [5]Energy Materials and Devices Key Laboratory of Anhui Province for Photoelectric Conversion,Anhui University,Hefei 230601,China

出　　处：《Rare Metals》2022年第5期1583-1594,共12页稀有金属（英文版）

基　　金：the National Science Foundation of China(No.12075002);the Outstanding Youth Fund of Anhui Province(No.2008085J21);Anhui Provincial Supporting Program for Excellent Young Talents in Universities(No.gxyqZD2019005);the Innovation and Entrepreneurship Project of Overseas Returnees in Anhui Province(No.2019LCX018)。

摘　　要：Energy-saving glycerol electrolysis with lower potential than water spitting endows a promising way for the concurrent production of value-added formate and high-purity hydrogen. However, there is still lack of efficient electrocatalysts at both anode and cathode for glycerol electrolysis. Herein, we report the activation of Ni site in NiV layered double hydroxide(LDH) by electrochemical and N_(2)/H_(2) plasma regulations for boosting the activity of glycerol oxidation reaction(GOR) and hydrogen evolution reaction(HER), respectively. Specifically, boosted GOR performance with a low overpotential(1.23 V at 10 mA·cm^(-2)) and a high Faradic efficiency(94%) is demonstrated by electrochemically regulated NiV LDH(ENiV LDH) with elevated valence state of Ni site. In situ Raman spectrum reveals the generation of Ni(Ⅲ) species by electrochemical regulation, and the highly active Ni(Ⅲ)can be regenerated with the process of electrochemical oxidation. Additionally, the possible reaction pathway is speculated based on the in situ Fourier transform infrared spectroscopy(FTIR) and high-performance liquid chromatography results. The plasma-regulated NiV LDH(PNiV LDH) with lower valence state of Ni site exhibits outstanding HER activity, displaying a low overpotential of 45 m V to deliver 10 mA·cm^(-2).When employing E-NiV LDH and P-NiV LDH as anode and cathode electrocatalyst, respectively, the assembled electrolyzer merely needs 1.25 V to achieve 10 m A·cm^(-2) for simultaneous production of formate and hydrogen, demonstrating remarkable 320 mV of lower potential than water electrolysis.

关 键 词：Glycerol electrolysis Glycerol oxidation reaction Hydrogen evolution reaction NiV LDH FORMATE 

分 类 号：TQ225.21[化学工程—有机化工] TQ116.2TQ426