Interatomic Electronegativity Offset Dictates Selectivity When Catalyzing the CO_2 Reduction Reaction

Jican Hao; Zechao Zhuang; Jiace HaoChan WangShuanglong LuFang DuanFangping XuMingliang DuHan Zhu

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Interatomic Electronegativity Offset Dictates Selectivity When Catalyzing the CO_2 Reduction Reaction

机译：Interatomic Electronegativity Offset Dictates Selectivity When Catalyzing the CO_2 Reduction Reaction

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Achieving efficient efficiency and selectivity for the electroreduction of CO_2to value-added feedstocks has been challenging, due to the thermodynamicstability of CO_2 molecules and the competing hydrogen evolution reaction.Herein, a dual-single-atom catalyst consisting of atomically dispersed CuN_4and NiN_4 bimetal sites is synthesized with electrospun carbon nanofibers(CuNi-DSA/CNFs). Theoretical and experimental studies reveal the strongelectron interactions induced by the electronegativity offset between the Cuand Ni atoms. The delicately averaged and compensated electronic structuresresult in an offset effect that optimizes the adsorption strength of the *COOHintermediate and boosts the CO_2 reduction reaction (CO_2RR) kinetics, notablypromoting the intrinsic activity and selectivity of the catalyst. The CuNi-DSA/CNFs catalyst exhibits an outstanding FECO of 99.6 across a broad potentialwindow of ?0.78- ?1.18 V (vs the reversible hydrogen electrode), a highturnover frequency of 2870 h-1, and excellent durability (25 h). Furthermore,an aqueous Zn-CO_2 battery for CO_2 power conversion is constructed. Thisatomic-level electronegativity offset of the dual-atom structures provides anappealing direction to develop advanced electrocatalysts for the CO_2RR.

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来源
《Advanced energy materials》 |2022年第26期|2200579.1-2200579.11|共11页
作者
Jican Hao; Zechao Zhuang; Jiace HaoChan WangShuanglong LuFang DuanFangping XuMingliang DuHan Zhu;
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作者单位

Key Laboratory of Synthetic and Biological ColloidsMinistry of EducationSchool of Chemical and Material EngineeringJiangnan UniversityWuxi, Jiangsu 214122, P. R. China;

Department of ChemistryTsinghua UniversityBeijing 100084, P. R. China;

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CO_2 electroreduction reaction; dual single atoms; electrospun nanofibers; interatomic electronegativity compensation;

Interatomic Electronegativity Offset Dictates Selectivity When Catalyzing the CO_2 Reduction Reaction

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