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Revealing the Kinetic Balance between Proton-Feeding and Hydrogenation in CO2 Electroreduction
Small ( IF 13.0 ) Pub Date : 2023-02-23 , DOI: 10.1002/smll.202300581
Sha Bai 1 , Ling Tan 1 , Chenjun Ning 1 , Guihao Liu 1 , Zhaohui Wu 1 , Tianyang Shen 1 , Lirong Zheng 2 , Yu-Fei Song 1
Affiliation  

Electrocatalytic reduction of CO2 to high-value-added chemicals provides a feasible path for global carbon balance. Herein, the fabrication of NiNPx@NiSAy-NG (x,y = 1, 2, 3; NG = nitrogen-doped graphite) is reported, in which Ni single atom sites (NiSA) and Ni nanoparticles (NiNP) coexist. These NiNPx@NiSAy-NG presented a volcano-like trend for maximum CO Faradaic efficiency (FECO) with the highest point at NiNP2@NiSA2-NG in CO2RR. NiNP2@NiSA2-NG exhibited ≈98% of maximum FECO and a large current density of −264 mA cm−2 at −0.98 V (vs. RHE) in the flow cell. In situ experiment and density functional theory (DFT) calculations confirmed that the proper content of NiSA and NiNP balanced kinetic between proton-feeding and CO2 hydrogenation. The NiNP in NiNP2@NiSA2-NG promoted the formation of H* and reduced the energy barrier of *CO2 hydrogenation to *COOH, and CO desorption can be efficiently facilitated by NiSA sites, thereby resulting in enhanced CO2RR performance.

中文翻译:

揭示 CO2 电还原中质子供给和氢化之间的动力学平衡

CO 2电催化还原为高附加值化学品为全球碳平衡提供了可行途径。在此,报道了 Ni NP x @Ni SA y -NG ( x,y  = 1, 2, 3; NG = 氮掺杂石墨) 的制备,其中 Ni 单原子位点 (Ni SA ) 和 Ni 纳米颗粒 (Ni NP)并存。这些 Ni NP x @Ni SA y -NG 呈现出最大 CO 法拉第效率 (FE CO )的火山样趋势,最高点在 CO 2 RR中的 Ni NP2 @Ni SA2 -NG 。Ni NP2 @NiSA2 -NG在流通池中表现出约 98% 的最大 FE CO和 -264 mA cm -2的大电流密度(-0.98 V(相对于 RHE))。原位实验和密度泛函理论(DFT) 计算证实,Ni SA和Ni NP的适当含量在质子供给和CO 2加氢之间平衡了动力学。Ni NP2 @Ni SA2 -NG中的Ni NP促进了 H* 的形成并降低了 *CO 2氢化为 *COOH的能垒,Ni SA位点可以有效促进 CO 解吸,从而提高 CO 2 RR表现。
更新日期:2023-02-23
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