Nitrogen-doped carbon (NC) for carbon dioxide reduction reaction (CORR) are promising candidates. However, its selectivity and activity are limited by the undeveloped pore and limited electronic effect. Herein, we propose a strategy of three birds with one stone to utilize the embedded nickel for inducing electron-rich pyridinic-NC with multimodal porous structure based on the hard template assisted sacrificial template method. Nickel acts as sacrificial agent and inducer to facilitate the formation of mesoporous and reactive nitrogen species for capturing and activating reactants, respectively. Besides, we find that nickel as electron donor endows the NC with electron accumulation for participating actively in PCET reaction. The resultant Ni-NC-1-AE exhibits an eminent FE of 97.6 % with excellent activity and stability. In-situ Raman spectroscopy and the projected crystal orbital Hamilton populations (pCOHP) confirm the accumulation of *COOH and the stable adsorption of *COOH on the surface. What’s more, the well-designed experiments and DFT calculations accurately locate pyridinic-N as the active site, where the aggregated electrons donated by nickel significantly reduce the energy barrier of rate-determining step and promote the desorption of CO. This work provides an instructive perspective to construct advanced NC electrocatalysts with high mass transfer efficiency and high catalytic activity.

中文翻译：

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嵌入金属诱导多介孔吡啶氮掺杂碳的电子积累，增强电化学 CO2 还原中 *COOH 的吸附

用于二氧化碳还原反应（CORR）的氮掺杂碳（NC）是有希望的候选者。然而，其选择性和活性受到不发达的孔隙和有限的电子效应的限制。在此，我们提出了一种基于硬模板辅助牺牲模板法的三鸟一石策略，利用嵌入的镍诱导具有多峰多孔结构的富电子吡啶-NC。镍充当牺牲剂和诱导剂，以促进介孔和活性氮物种的形成，分别用于捕获和活化反应物。此外，我们发现镍作为电子给体赋予NC电子积累，从而积极参与PCET反应。所得 Ni-NC-1-AE 的 FE 高达 97.6%，具有优异的活性和稳定性。原位拉曼光谱和投影晶体轨道汉密尔顿布居 (pCOHP) 证实了 *COOH 的积累和 *COOH 在表面上的稳定吸附。此外，精心设计的实验和DFT计算准确地将吡啶-N定位为活性位点，镍提供的聚集电子显着降低了速率决定步骤的能垒，促进了CO的解吸。这项工作提供了指导性的指导。构建具有高传质效率和高催化活性的先进NC电催化剂。