部分
材料科学
多物理
电化学
密度泛函理论
钴
吸附
分子
催化作用
化学工程
纳米技术
电极
物理化学
计算化学
化学
有限元法
立体化学
热力学
冶金
有机化学
物理
工程类
作者
Shanhe Gong,Shuo Yang,Wenbo Wang,Runqing Lu,Haotan Wang,Xu Han,Guilong Wang,Jimin Xie,Dewei Rao,Chunxia Wu,Jun Li,Shouyan Shao,Xiaomeng Lv
出处
期刊:Small
[Wiley]
日期:2023-03-21
卷期号:19 (26)
被引量:2
标识
DOI:10.1002/smll.202207808
摘要
Optimizing the coordination structure and microscopic reaction environment of isolated metal sites is promising for boosting catalytic activity for electrocatalytic CO2 reduction reaction (CO2 RR) but is still challenging to achieve. Herein, a newly electrostatic induced self-assembly strategy for encapsulating isolated Ni-C3 N1 moiety into hollow nano-reactor as I-Ni SA/NHCRs is developed, which achieves FECO of 94.91% at -0.80 V, the CO partial current density of ≈-15.35 mA cm-2 , superior to that with outer Ni-C2 N2 moiety (94.47%, ≈-12.06 mA cm-2 ), or without hollow structure (92.30%, ≈-5.39 mA cm-2 ), and high FECO of ≈98.41% at 100 mA cm-2 in flow cell. COMSOL multiphysics finite-element method and density functional theory (DFT) calculation illustrate that the excellent activity for I-Ni SA/NHCRs should be attributed to the structure-enhanced kinetics process caused by its hollow nano-reactor structure and unique Ni-C3 N1 moiety, which can enrich electron on Ni sites and positively shift d-band center to the Fermi level to accelerate the adsorption and activation of CO2 molecule and *COOH formation. Meanwhile, this strategy also successfully steers the design of encapsulating isolated iron and cobalt sites into nano-reactor, while I-Ni SA/NHCRs-based zinc-CO2 battery assembled with a peak power density of 2.54 mW cm--2 is achieved.
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