Fine-tuning inverse metal-support interaction boosts electrochemical transformation of methanol into formaldehyde based on density functional theory
Fine-tuning inverse metal-support interaction boosts electrochemical transformation of methanol into formaldehyde based on density functional theory
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基于密度泛函理论微调逆金属-载体相互作用促进甲醇电化学转化为甲醛
DOI：
10.1016/j.cclet.2020.12.057
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发表时间：
2021-01
影响因子：
9.1
通讯作者：
Zhang Qitao
中科院分区：
文献类型：
--
作者：
Yang Wenjuan;Li Junjun;Cui Xiaoya;Yang Chenhuai;Liu Yiting;Zeng Xianwei;Zhang Zhicheng;Zhang Qitao
与传统的金属载体多相催化剂不同，以金属氧化物修饰金属表面的反相多相催化剂，由于其独特的界面效应和电子结构，近年来引起了人们越来越多的兴趣。然而，深入了解金属-氧化物相互作用对催化性能的影响仍然是一个巨大的挑战。在我们的工作中，一种反赤铁矿/钯(Fe2O3/Pd)杂化纳米结构，即部分覆盖在Pd纳米颗粒(NPs)表面的活性Fe2O3超薄氧化层，基于密度泛函理论计算，显示出比裸Pd纳米颗粒对甲醇氧化反应(MOR)更好的电催化性能。在Pd/Fe_2O_3界面内建电势的驱动下，电荷可以从Pd向Fe_2O_3转移，有利于Pd能带中心的下移。在界面羟基OH的辅助下，CH3OH中的单键H和单键H的断裂更容易发生，在Fe_2O_3/Pd上的势垒比在纯Pdviato两个电子转移反应通道上低得多。结果表明，界面处Pd和Fe2O_3的协同作用可以促进甲醇在界面羟基OH~*辅助下电化学转化为甲醛。
Different from traditional metal-support heterogenous catalysts, inverse heterogeneous catalysts, in which the surface of metal is decorated by metal oxide, have recently attracted increasing interests owing to the unique interfacial effect and electronic structure. However, a deep insight into the effect of metal-oxide interaction on the catalytic performance still remains a great challenge. In our work, an inverse hematite/palladium (Fe2O3/Pd) hybrid nanostructure,i.e., the active Fe2O3ultrathin oxide layers partially covering on the surface of Pd nanoparticles (NPs), exhibited superior electrocatalytic performance towards methanol oxidation reaction (MOR) as compared to the bare Pd NPs based on density functional theory calculation. The charge could transfer from Pd to Fe2O3driven by the built-in potential at the interface of Pd and Fe2O3, which favors the downshift ofdband center of Pd. With the assistance of interfacial hydroxyl OH*, the cleavage of Osingle bondH and Csingle bondH in CH3OH could take place much easily with lower barrier energy on Fe2O3/Pd than that on pure Pdviatwo electrons transferring reaction pathways. Our results highlight that the synergy of Pd and Fe2O3at the interface could facilitate the electrochemical transformation of methanol into formaldehyde assisted with interfacial hydroxyl OH*.
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影响因子：
5
作者：
Fenglin Liao;T. W. Benedict Lo;Jin Qu;A. Kroner;A. Dent;S. Tsang
通讯作者：
Fenglin Liao;T. W. Benedict Lo;Jin Qu;A. Kroner;A. Dent;S. Tsang
一步合成用于甲醇氧化反应的成分可控的PdPt双金属纳米枝晶
影响因子：
8.1
作者：
Yuan Zhang;Jinfeng Zhang;Zelin Chen;Yunwei Liu;Mengmeng Zhang;Xiaopeng Han;Cheng Zhong;Wenbin Hu;Yida Deng
通讯作者：
Yida Deng
超薄但可转移的 Pt 或 PtRu 装饰石墨烯薄膜作为甲醇氧化反应的有效电催化剂
影响因子：
8.1
作者：
Tao Zhuchen;Chen Wei;Yang Jing;Wang Xiangyang;Tan Ziqi;Ye Jianglin;Chen Yanxia;Zhu Yanwu
通讯作者：
Zhu Yanwu
影响因子：
15
作者：
Liu, Xiaoyan;Liu, Ming-Han;Lin, Tien-Sung
通讯作者：
Lin, Tien-Sung
影响因子：
5.7
作者：
Kim, Hyun You;Henkelman, Graeme
通讯作者：
Henkelman, Graeme