Harmonizing the Electronic Structures of the Adsorbate and Catalysts for Efficient CO2 Reduction
Harmonizing the Electronic Structures of the Adsorbate and Catalysts for Efficient CO2 Reduction
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协调吸附物和催化剂的电子结构以有效减少二氧化碳
DOI：
10.1021/acs.nanolett.9b02782
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发表时间：
2019
期刊：
影响因子：
10.8
通讯作者：
Zeng Jie
中科院分区：
文献类型：
--
作者：
Zhang An;Liang Yongxiang;Li Huiping;Zhao Xinyu;Chen Yuliang;Zhang Boyan;Zhu Wenguang;Zeng Jie
CO2电还原的关键瓶颈在于CO2的活化，其需要高的过电位。CO2的活化与催化剂和吸附质的电子结构有关，理想的催化剂应与吸附质的电子结构相匹配。在这里，我们协调的吸附物和Mn掺杂的In 2S 3纳米片的电子结构，有效的CO2还原。在In 2S 3纳米片中引入Mn掺杂剂提高了碳质产物的法拉第效率（FE）和电流密度（j）。在-0.9 V vs. RHE下，Mn掺杂的In 2S 3纳米片在20.1 mA cm-2的高J下对碳质产物表现出92%的显著FE。机理研究表明，在CO2活化过程中，Mn掺杂使Mn掺杂In 2S 3纳米片导带边缘附近的O原子轨道和Mn原子轨道之间发生谐波重叠。由于共吸附构型的独特电子结构，Mn掺杂的In 2S 3纳米片表现出低于原始In 2S 3纳米片的CO2活化成HCOO* 的能垒。
In CO2electroreduction, the critical bottleneck lies in the CO2activation which requires high overpotentials. CO2activation is related to both the electronic structures of catalysts and those of adsorbates, thus an ideal catalyst should match its electronic structures with those of the adsorbate. Here, we harmonized the electronic structures of the adsorbate and Mn-doped In2S3nanosheets for efficient CO2reduction. The introduction of Mn dopants into In2S3nanosheets enhanced both the Faradaic efficiency (FE) for carbonaceous products and current density (j). At −0.9 V vs RHE, Mn-doped In2S3nanosheets exhibited a remarkable FE of 92% for carbonaceous product at a highjof 20.1 mA cm–2. Mechanistic studies revealed that Mn doping enabled the harmonic overlaps between theporbitals of O atoms anddorbitals of Mn atoms near the conduction band edge of Mn-doped In2S3nanosheets during the activation of CO2. Due to the unique electronic structures of the coadsorbed configurations, Mn-doped In2S3nanosheets exhibited an energy barrier for CO2activation into HCOO* lower than that over pristine In2S3nanosheets.