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负载型Pd2双原子位催化剂用于高效电化学CO2还原
作者:小柯机器人 发布时间:2021/4/7 13:36:35

清华大学王定胜团队合成了负载型Pd2双原子位催化剂并首次用于电化学CO2还原反应。相关研究成果于2021年4月4日发表于国际顶尖学术期刊《德国应用化学》。

双原子位催化剂(DACs)在保持单原子位催化剂(SACs)100%的原子利用率和优良的选择性的同时,由于相邻金属原子间的协同作用,提高了催化剂的催化活性,成为多相催化领域的一个新前沿。

该文首次合成了负载型Pd2 DAC,并将其用于电化学Co2还原反应(Co2-RR)。所获得的Pd 2 DAC在0.85 V下表现出优异的CO 2 RR催化性能,与RHE相比,具有98.2%FE CO,远远超过Pd1 SAC,并且具有长期稳定性。

密度泛函理论(DFT)计算表明,Pd-2DAC对Co2-RR具有较高活性的内在原因是Pd二聚体中Pd原子间的电子转移。因此,Pd2 DAC对CO*的吸附强度适中,有利于Co2-RR中CO的生成。

附:英文原文

Title: Supported Pd2 Dual‐atom Site Catalyst for Efficient Electrochemical CO2 Reduction

Author: Ningqiang Zhang, Xinxin Zhang, Yikun Kang, Chenliang Ye, Rui Jin, Han Yan, Rui Lin, Jiarui Yang, Qian Xu, Yu Wang, Qinghua Zhang, Lin Gu, Licheng Liu, Weiyu Song, Jian Liu, Dingsheng Wang, Yadong Li

Issue&Volume: 2021-04-04

Abstract: Dual‐atom site catalysts (DACs) have emerged as a new frontier in heterogeneous catalysis because the synergistic effect between adjacent metal atoms can promote their catalytic activity while maintaining the advantages of single‐atom site catalysts (SACs), like 100% atomic utilization efficiency and excellent selectivity. Herein, a supported Pd 2  DAC was synthesized and used for electrochemical CO 2  reduction reaction (CO 2  RR) for the first time. The as‐obtained Pd 2  DAC exhibited superior CO 2  RR catalytic performance with 98.2% FE CO  at ‐0.85 V vs. RHE, far exceeding that of Pd 1  SAC, and coupled with long‐term stability. The density functional theory (DFT) calculations revealed that the intrinsic reason for the superior activity of Pd 2  DAC toward CO 2  RR was the electron transfer between Pd atoms at the dimeric Pd sites. Thus, Pd 2  DAC possessed moderate adsorption strength of CO*, which was beneficial for CO production in CO 2  RR.

DOI: 10.1002/anie.202101559

Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.202101559

期刊信息

Angewandte Chemie:《德国应用化学》,创刊于1887年。隶属于德国化学会,最新IF:12.959
官方网址:https://onlinelibrary.wiley.com/journal/15213773
投稿链接:https://www.editorialmanager.com/anie/default.aspx