首页|A cascade of in situ conversion of bicarbonate to CO2 and CO2 electroreduction in a flow cell with a Ni-N-S catalyst

A cascade of in situ conversion of bicarbonate to CO2 and CO2 electroreduction in a flow cell with a Ni-N-S catalyst

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Combination of CO2 capture using inorganic alkali with subsequently electrochemical conversion of the resultant HCO3-to high-value chemicals is a promising route of low cost and high efficiency.The electro-chemical reduction of HCO3-is challenging due to the inaccessible of negatively charged molecular groups to the electrode surface.Herein,we adopt a comprehensive strategy to tackle this challenge,i.e.,cascade of in situ chemical conversion of HCO3-to CO2 and CO2 electrochemical reduction in a flow cell.With a tailored Ni-N-S single atom catalyst(SACs),where sulfur(S)atoms located in the second shell of Ni cen-ter,the CO2 electroreduction(CO2ER)to CO is boosted.The experimental results and density functional theory(DFT)calculations reveal that the introduction of S increases the p electron density of N atoms near Ni atom,thereby stabilizing*H over N and boosting the first proton coupled electron transfer pro-cess of CO2ER,i.e.,*+e-+*H+*CO2→*COOH.As a result,the obtained catalyst exhibits a high faradaic effi-ciency(FEco～98％)and a low overpotential of 425 mV for CO production as well as a superior turnover frequency(TOF)of 47397 h-1,outcompeting most of the reported Ni SACs.More importantly,an extre-mely high FEco of 90％is achieved at 50 mA cm-2 in the designed membrane electrode assembly(MEA)cascade electrolyzer fed with liquid bicarbonate.This work not only highlights the significant role of the second coordination on the first coordination shell of the central metal for CO2ER,but also provides an alternative and feasible strategy to realize the electrochemical conversion of HCO3-to high-value chemicals.

S doped Ni-N-C single atom catalystsCO2 electrochemical reductionDFT calculationsMembrane electrode assemblyReduction of bicarbonate

Linghui Kong、Min Wang、Yongxiao Tuo、Shanshan Zhou、Jinxiu Wang、Guangbo Liu、Xuejing Cui、Jiali Wang、Luhua Jiang

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Nanomaterials and Electrocatalysis Laboratory,College of Materials Science and Engineering,Qingdao University of Science and Technology,Qingdao 266042,Shandong,China

State Key Laboratory of Heavy Oil Processing,College of New Energy,China University of Petroleum(East China),Qingdao 266580,Shandong,China

Natural Science Foundation of Shandong ProvinceNatural Science Foundation of Shandong ProvinceOpening Project of State Key Laboratory of High Performance Ceramics and Superfine MicrostructureTaishan Scholar Program of Shandong Province

ZR2020QB132ZR2020MB025SKL202108SICts201712046

2024

10.1016/j.jechem.2023.09.024

能源化学
中国科学院大连化学物理研究所 中国科学院成都有机化学研究所

能源化学

CSTPCDEI
影响因子：0.654
ISSN：2095-4956
年,卷(期)：2024.88(1)
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