Evaluating Metal-Support Interaction in Formaldehyde Oxidation Using Pd/TiO2 Catalysts: The Key Role of Mono-Oxygen Vacancies.

IF 4.7 2区化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR

Inorganic Chemistry Pub Date : 2025-05-14 DOI:10.1021/acs.inorgchem.5c00586

Xudong Chen,Chunying Wang,Jingyi Wang,Wei Wen,Xiaofeng Liu,Yaobin Li,Wenpo Shan,Hong He

{"title":"Evaluating Metal-Support Interaction in Formaldehyde Oxidation Using Pd/TiO2 Catalysts: The Key Role of Mono-Oxygen Vacancies.","authors":"Xudong Chen,Chunying Wang,Jingyi Wang,Wei Wen,Xiaofeng Liu,Yaobin Li,Wenpo Shan,Hong He","doi":"10.1021/acs.inorgchem.5c00586","DOIUrl":null,"url":null,"abstract":"Metal-support interactions (MSI) have been widely recognized as playing a key role in regulating the catalytic activity in various reactions. However, clarifying the relationship linking catalyst defect structures, active sites, and catalytic performance for catalysts with a constructed MSI remains a challenge. Here, Pd/TiO2 catalysts with adjustable MSI were designed and fabricated based on defect engineering. Comprehensive characterization analysis revealed that as the catalyst reduction temperature and defect content increase, the MSI gradually increases, subsequently enhancing the intrinsic activity of the catalyst to oxidize formaldehyde (HCHO). However, the activity of the catalyst exhibited a volcano-shaped trend, which was caused by the collapse of the support structure at a high reduction temperature. Through comparative analysis of the HCHO oxidation reaction and CO oxidation reaction activity tests, it was confirmed that the ratio of mono-oxygen vacancies to oxygen vacancy clusters (I1/I2) in this study system could reliably serve as a valid \"descriptor\" for HCHO oxidation apparent activity.","PeriodicalId":40,"journal":{"name":"Inorganic Chemistry","volume":"57 1","pages":""},"PeriodicalIF":4.7000,"publicationDate":"2025-05-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Inorganic Chemistry","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/acs.inorgchem.5c00586","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, INORGANIC & NUCLEAR","Score":null,"Total":0}

引用次数: 0

Abstract

Metal-support interactions (MSI) have been widely recognized as playing a key role in regulating the catalytic activity in various reactions. However, clarifying the relationship linking catalyst defect structures, active sites, and catalytic performance for catalysts with a constructed MSI remains a challenge. Here, Pd/TiO2 catalysts with adjustable MSI were designed and fabricated based on defect engineering. Comprehensive characterization analysis revealed that as the catalyst reduction temperature and defect content increase, the MSI gradually increases, subsequently enhancing the intrinsic activity of the catalyst to oxidize formaldehyde (HCHO). However, the activity of the catalyst exhibited a volcano-shaped trend, which was caused by the collapse of the support structure at a high reduction temperature. Through comparative analysis of the HCHO oxidation reaction and CO oxidation reaction activity tests, it was confirmed that the ratio of mono-oxygen vacancies to oxygen vacancy clusters (I1/I2) in this study system could reliably serve as a valid "descriptor" for HCHO oxidation apparent activity.

查看原文本刊更多论文

用Pd/TiO2催化剂评价甲醛氧化过程中金属-载体相互作用：单氧空位的关键作用。

金属-载体相互作用（MSI）在调节各种反应的催化活性中起着重要作用。然而，澄清催化剂缺陷结构、活性位点和催化剂的催化性能与构建的MSI之间的关系仍然是一个挑战。本文以缺陷工程为基础，设计并制备了MSI可调的Pd/TiO2催化剂。综合表征分析发现，随着催化剂还原温度和缺陷含量的增加，MSI逐渐增加，从而增强了催化剂氧化甲醛（HCHO）的固有活性。然而，催化剂的活性呈现火山状趋势，这是由于支撑结构在高还原温度下坍塌造成的。通过对HCHO氧化反应和CO氧化反应活性测试的对比分析，证实了本研究体系中单氧空位与氧空位簇的比值（I1/I2）可以可靠地作为HCHO氧化表观活性的有效“描述符”。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

求助全文

约1分钟内获得全文求助全文

来源期刊

Inorganic Chemistry 化学-无机化学与核化学

CiteScore

7.60

自引率

13.00%

发文量

1960

审稿时长

1.9 months

期刊介绍： Inorganic Chemistry publishes fundamental studies in all phases of inorganic chemistry. Coverage includes experimental and theoretical reports on quantitative studies of structure and thermodynamics, kinetics, mechanisms of inorganic reactions, bioinorganic chemistry, and relevant aspects of organometallic chemistry, solid-state phenomena, and chemical bonding theory. Emphasis is placed on the synthesis, structure, thermodynamics, reactivity, spectroscopy, and bonding properties of significant new and known compounds.