Microenvironment Engineering of Single/Dual‐Atom Catalysts for Electrocatalytic Application

Gao, Yun.; Liu, Baozhong; Wang, Dingsheng

doi:10.1002/adma.202209654

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Microenvironment Engineering of Single/Dual‐Atom Catalysts for Electrocatalytic Application

Author(s): Yun Gao ¹ , Baozhong Liu ² , Dingsheng Wang ¹

Publication date (Electronic): June 28 2023

Journal: Advanced Materials

Publisher: Wiley

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Abstract

Single/dual‐metal atoms supported on carbon matrix can be modulated by coordination structure and neighboring active sites. Precisely designing the geometric and electronic structure and uncovering the structure–property relationships of single/dual‐metal atoms confront with grand challenges. Herein, this review summarizes the latest progress in microenvironment engineering of single/dual‐atom active sites via a comprehensive comparison of single‐atom catalyst (SACs) and dual‐atom catalysts (DACs) in term of design principles, modulation strategy, and theoretical understanding of structure–performance correlations. Subsequently, recent advances in several typical electrocatalysis process are discussed to get general understanding of the reaction mechanisms on finely‐tuned SACs and DACs. Finally, full‐scaled summaries of the challenges and prospects are given for microenvironment engineering of SACs and DACs. This review will provide new inspiration on the development of atomically dispersed catalysts for electrocatalytic application.

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Combining theory and experiment in electrocatalysis: Insights into materials design

Zhi Seh, Jakob Kibsgaard, Colin F. Dickens … (2017)

Electrocatalysis plays a central role in clean energy conversion, enabling a number of sustainable processes for future technologies. This review discusses design strategies for state-of-the-art heterogeneous electrocatalysts and associated materials for several different electrochemical transformations involving water, hydrogen, and oxygen, using theory as a means to rationalize catalyst performance. By examining the common principles that govern catalysis for different electrochemical reactions, we describe a systematic framework that clarifies trends in catalyzing these reactions, serving as a guide to new catalyst development while highlighting key gaps that need to be addressed. We conclude by extending this framework to emerging clean energy reactions such as hydrogen peroxide production, carbon dioxide reduction, and nitrogen reduction, where the development of improved catalysts could allow for the sustainable production of a broad range of fuels and chemicals.

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Single-atom catalysis of CO oxidation using Pt1/FeOx.

Botao Qiao, Aiqin Wang, Xiaofeng Yang … (2011)

Platinum-based heterogeneous catalysts are critical to many important commercial chemical processes, but their efficiency is extremely low on a per metal atom basis, because only the surface active-site atoms are used. Catalysts with single-atom dispersions are thus highly desirable to maximize atom efficiency, but making them is challenging. Here we report the synthesis of a single-atom catalyst that consists of only isolated single Pt atoms anchored to the surfaces of iron oxide nanocrystallites. This single-atom catalyst has extremely high atom efficiency and shows excellent stability and high activity for both CO oxidation and preferential oxidation of CO in H2. Density functional theory calculations show that the high catalytic activity correlates with the partially vacant 5d orbitals of the positively charged, high-valent Pt atoms, which help to reduce both the CO adsorption energy and the activation barriers for CO oxidation.