期刊
CHEMOSPHERE
卷 291, 期 -, 页码 -出版社
PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.chemosphere.2021.132889
关键词
Hydrocerussite; Electrocatalyst; Electrochemical CO2 reduction; HCOOH; MOFs; Surface defects
资金
- Zhejiang Provincial Natural Science Foundation of China [LZ18B070001, LQ21E080011]
- China Postdoctoral Science Foundation [2021M693414]
- National Natural Science Foundation of China [22076168, 52000158, 22006131, 21908199, 51978654, 21876156]
- Zhejiang Provincial Ten Thousand Talent Program [2018R52013]
- Central Government Guided Local Science and Technology Development Fund [2021ZY1022]
A metal oxide electrode has been developed for electrochemical CO2 reduction reaction, exhibiting superior activity and product selectivity. By synthesizing a hydrocerussite thin film on a Pb substrate, the electrode shows high selectivity and activity towards formic acid production.
A metal oxide electrode has been developed for the electrochemical CO2 reduction reaction (eCO(2)RR). It exhibits superior activity and product selectivity towards eCO(2)RR by circumventing the previously encountered problem of self-reduction with high-valence metals. Specifically, a hydrocerussite [Pb-3(CO3)(2)(OH)(2)] thin film has been synthesized in situ on a Pb substrate (denoted as ER-HC) by an electroreduction method using a lead-based metal-organic framework (Pb-MOF) as a precursor. The ER-HC electrode exhibits a high selectivity of 96.8% towards HCOOH production with a partial current density of 1.9 mA cm-2 at-0.88 V vs. the reversible hydrogen electrode (RHE). A higher HCOOH partial current density of 7.3 mA cm(-2) has been achieved at-0.98 V vs. RHE. Physicochemical and electrochemical characterization results demonstrate that the defective hydrocerussite surface exhibits appropriate adsorption free energy of formate (HCOO-) and a lower reaction free energy for HCOOH production from CO2, which greatly boosts the eCO(2)RR activity and HCOOH production selectivity. The structure and eCO(2)RR performance of the hydrocerussite thin film remain stable in 0.1 M KHCO3 as electrolyte, ensuring its durability. Overall, this work not only provides a metal oxide electrode (metal hydroxide, to be more precise) with excellent eCO(2)RR performance, but also expands the in situ electrochemical derivatization strategy for the fabrication of metal oxide electrodes.
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