PtCu-a-SnO2 interface engineering on PtCu-SnO2 aerogels for ethanol oxidation electrocatalysis

IF 13.3 1区 工程技术 Q1 ENGINEERING, CHEMICAL Chemical Engineering Journal Pub Date : 2024-10-02 DOI:10.1016/j.cej.2024.156321
Yongying Wang, Yangge Guo, Zhengwei Zhang, Zirui Wu, Chanez Maouche, Shuiyun Shen, Yi Li, Junliang Zhang, Juan Yang
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Abstract

Designing catalysts with high activity and stability to boost their ethanol oxidation reaction (EOR) performance is one of the central targets in the development of direct ethanol fuel cells (DEFCs). However, how to design the EOR catalysts in a rational way is still challenging, needing more efforts put in. Herein, we have synthesized a catalyst of PtCu-SnO2 aerogel via ingeniously introducing Cu into Pt-SnO2 system, resulting in the formation of a main phase of alloy (PtCu)-amorphous oxide (a-SnO2) interface. Benefiting from the optimized structures, the PtCu-SnO2 aerogel displays excellent acidic EOR performance with 4.5 times promotion in activity compared to pure Pt aerogel. In-depth investigations through electrochemical in-situ Fourier transform infrared spectroscopy and density functional theory calculations have shown that the absorbed OH on a-SnO2 surface together with the greatly-modified electronic structure of the alloy surface atoms can facilitate the C1 pathway and the oxidation of *CO intermediates for ethanol oxidation reaction. The resulting affinity of surface OH and the modification of reaction energies both in turn contribute to the improvement of EOR performance with high activity, stability, and anti-poisoning ability, proving interfacial engineering an effective strategy for the rational design of EOR catalyst.

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用于乙醇氧化电催化的 PtCu-SnO2 气凝胶上的 PtCu-a-SnO2 界面工程
设计具有高活性和稳定性的催化剂以提高其乙醇氧化反应(EOR)性能,是开发直接乙醇燃料电池(DEFC)的核心目标之一。然而,如何合理地设计乙醇氧化反应催化剂仍然具有挑战性,需要付出更多的努力。在此,我们通过在 Pt-SnO2 体系中巧妙地引入铜,形成合金(PtCu)-非晶态氧化物(a-SnO2)界面主相,合成了 PtCu-SnO2 气凝胶催化剂。得益于优化的结构,PtCu-SnO2 气凝胶显示出优异的酸性 EOR 性能,其活性比纯铂气凝胶提高了 4.5 倍。通过电化学原位傅立叶变换红外光谱和密度泛函理论计算进行的深入研究表明,a-SnO2 表面吸收的 OH 与合金表面原子电子结构的大幅改良可促进乙醇氧化反应的 C1 通路和 *CO 中间产物的氧化。由此产生的表面 OH 亲和力和反应能的改变反过来又有助于提高 EOR 性能,使其具有高活性、稳定性和抗中毒能力,从而证明界面工程是合理设计 EOR 催化剂的有效策略。
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来源期刊
Chemical Engineering Journal
Chemical Engineering Journal 工程技术-工程:化工
CiteScore
21.70
自引率
9.30%
发文量
6781
审稿时长
2.4 months
期刊介绍: The Chemical Engineering Journal is an international research journal that invites contributions of original and novel fundamental research. It aims to provide an international platform for presenting original fundamental research, interpretative reviews, and discussions on new developments in chemical engineering. The journal welcomes papers that describe novel theory and its practical application, as well as those that demonstrate the transfer of techniques from other disciplines. It also welcomes reports on carefully conducted experimental work that is soundly interpreted. The main focus of the journal is on original and rigorous research results that have broad significance. The Catalysis section within the Chemical Engineering Journal focuses specifically on Experimental and Theoretical studies in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. These studies have industrial impact on various sectors such as chemicals, energy, materials, foods, healthcare, and environmental protection.
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