Asymmetric coordinative modulation boosting the activity and thermal stability of Pt1/CeO2 for CO oxidation under harsh condition

IF 13.3 1区工程技术 Q1 ENGINEERING, CHEMICAL

Chemical Engineering Journal Pub Date : 2024-11-07 DOI:10.1016/j.cej.2024.157250

Lijun Ni , Yuwei Zhou , Wei Tan , Hong Li , Dong Wang , Qi Zhang , Bing Yang , Jing Xu , Ying Zhang , Chengsi Pan , Yongfa Zhu , Fudong Liu , Yang Lou

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Abstract

Supported metal catalysts play a central role in chemical industry, but it remains a formidable challenge to realize high activity while maintaining atomically dispersed status to maximize atom efficiency under harsh conditions. Herein, a novel strategy of constructing asymmetric coordination Pt active sites via coating N-doped carbon onto ceria supported Pt single atoms (Pt₁/CeO₂@CN) is proposed, through which superior low-temperature CO oxidation activity and satisfactory thermal stability are achieved simultaneously. Experimental and density functional theory results confirm that the unique asymmetric N₂-Pt₁-O₂ coordinative configuration on Pt₁/CeO₂@CN tailors the electronic properties of Pt 5d states, increasing the turnover frequency by 15 times for CO oxidation at 120 °C compared with that on Pt₁/CeO₂ and sustaining the atomically dispersed status of Pt at as high as 400 °C under H₂-containing atmosphere. This strategy suggests a promising avenue to fabricating highly active and stable supported metal catalysts for practical applications under harsh conditions.

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不对称配位调节提高了 Pt1/CeO2 在苛刻条件下氧化 CO 的活性/热稳定性

支撑金属催化剂在化学工业中发挥着重要作用，但如何在实现高活性的同时保持原子分散状态，从而在苛刻条件下最大限度地提高原子效率，仍是一项艰巨的挑战。本文提出了一种新策略，即通过在铈支撑铂单原子上包覆掺杂 N 的碳（Pt1/CeO2@CN）来构建不对称配位铂活性位点，从而同时获得优异的低温 CO 氧化活性和令人满意的热稳定性。实验和密度泛函理论结果证实，Pt1/CeO2@CN 独特的不对称 N2-Pt1-O2 配位构型调整了铂 5d 态的电子特性，与 Pt1/CeO2 相比，120 ℃ 下 CO 氧化的翻转频率提高了 15 倍，并且在含 H2- 的气氛下，铂的原子分散状态在高达 400 ℃ 时仍能保持。这一策略为制造高活性、高稳定性的支撑金属催化剂提供了一条在苛刻条件下实际应用的可行途径。

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来源期刊

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.