高效、选择性氧化催化剂中氢化Pt-Ce-H位点的形成。

IF 44.7 1区综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES

Science Pub Date : 2025-04-03 DOI:10.1126/science.adv0735

Ji Yang, Lorenz J. Falling, Siyang Yan, Biluan Zhang, Pragya Verma, Luke Daemen, Yongqiang Cheng, Xiao Zhao, Shuchen Zhang, Jeng-Lung Chen, Bingqing Yao, Shengdong Tan, Sudong Chae, Qian He, Slavomir Nemsak, Zili Wu, David Prendergast, Yanbing Guo, Jiaxu Liu, Miquel Salmeron, Ji Su

{"title":"高效、选择性氧化催化剂中氢化Pt-Ce-H位点的形成。","authors":"Ji Yang, Lorenz J. Falling, Siyang Yan, Biluan Zhang, Pragya Verma, Luke Daemen, Yongqiang Cheng, Xiao Zhao, Shuchen Zhang, Jeng-Lung Chen, Bingqing Yao, Shengdong Tan, Sudong Chae, Qian He, Slavomir Nemsak, Zili Wu, David Prendergast, Yanbing Guo, Jiaxu Liu, Miquel Salmeron, Ji Su","doi":"10.1126/science.adv0735","DOIUrl":null,"url":null,"abstract":"<div >Single-atom site catalysts can improve the rates and selectivity of many catalytic reactions. We have modified Pt1/CeO2 single sites by combining them with molecular groups and with oxygen vacancies of the support. The new sites include hydrided (Pt2+-Ce3+Hδ−) and hydroxylated (Pt2+-Ce3+OH) sites that exhibit higher reactivity and selectivity to previous single sites for several reactions, including a ninefold increase in the reaction rate for carbon monoxide oxidation and a 2.3-fold improvement of propylene selectivity for oxidative dehydrogenation of propane. The atomic structure and reaction steps of these sites were determined with in situ and ex situ spectroscopy techniques and theoretical methods.</div>","PeriodicalId":21678,"journal":{"name":"Science","volume":"388 6746","pages":""},"PeriodicalIF":44.7000,"publicationDate":"2025-04-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Formation of hydrided Pt-Ce-H sites in efficient, selective oxidation catalysts\",\"authors\":\"Ji Yang, Lorenz J. Falling, Siyang Yan, Biluan Zhang, Pragya Verma, Luke Daemen, Yongqiang Cheng, Xiao Zhao, Shuchen Zhang, Jeng-Lung Chen, Bingqing Yao, Shengdong Tan, Sudong Chae, Qian He, Slavomir Nemsak, Zili Wu, David Prendergast, Yanbing Guo, Jiaxu Liu, Miquel Salmeron, Ji Su\",\"doi\":\"10.1126/science.adv0735\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div >Single-atom site catalysts can improve the rates and selectivity of many catalytic reactions. We have modified Pt1/CeO2 single sites by combining them with molecular groups and with oxygen vacancies of the support. The new sites include hydrided (Pt2+-Ce3+Hδ−) and hydroxylated (Pt2+-Ce3+OH) sites that exhibit higher reactivity and selectivity to previous single sites for several reactions, including a ninefold increase in the reaction rate for carbon monoxide oxidation and a 2.3-fold improvement of propylene selectivity for oxidative dehydrogenation of propane. The atomic structure and reaction steps of these sites were determined with in situ and ex situ spectroscopy techniques and theoretical methods.</div>\",\"PeriodicalId\":21678,\"journal\":{\"name\":\"Science\",\"volume\":\"388 6746\",\"pages\":\"\"},\"PeriodicalIF\":44.7000,\"publicationDate\":\"2025-04-03\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Science\",\"FirstCategoryId\":\"103\",\"ListUrlMain\":\"https://www.science.org/doi/10.1126/science.adv0735\",\"RegionNum\":1,\"RegionCategory\":\"综合性期刊\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"MULTIDISCIPLINARY SCIENCES\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Science","FirstCategoryId":"103","ListUrlMain":"https://www.science.org/doi/10.1126/science.adv0735","RegionNum":1,"RegionCategory":"综合性期刊","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MULTIDISCIPLINARY SCIENCES","Score":null,"Total":0}

引用次数: 0

摘要

单原子位催化剂可以提高许多催化反应的速率和选择性。我们通过将Pt1/CeO2单位点与分子基团和载体的氧空位结合来修饰它们。新的位点包括氢化位点（Pt2+-Ce3+Hδ）和羟基化位点（Pt2+-Ce3+OH），这些位点在几个反应中表现出更高的反应活性和选择性，包括一氧化碳（CO）氧化反应速率提高9倍，丙烷氧化脱氢丙烯选择性提高2.3倍。用原位、非原位光谱技术和理论方法测定了这些位点的原子结构和反应步骤。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

查看原文本刊更多论文

Formation of hydrided Pt-Ce-H sites in efficient, selective oxidation catalysts

Single-atom site catalysts can improve the rates and selectivity of many catalytic reactions. We have modified Pt₁/CeO₂ single sites by combining them with molecular groups and with oxygen vacancies of the support. The new sites include hydrided (Pt²⁺-Ce³⁺H^δ−) and hydroxylated (Pt²⁺-Ce³⁺OH) sites that exhibit higher reactivity and selectivity to previous single sites for several reactions, including a ninefold increase in the reaction rate for carbon monoxide oxidation and a 2.3-fold improvement of propylene selectivity for oxidative dehydrogenation of propane. The atomic structure and reaction steps of these sites were determined with in situ and ex situ spectroscopy techniques and theoretical methods.

求助全文

通过发布文献求助，成功后即可免费获取论文全文。去求助

来源期刊

Science 综合性期刊-综合性期刊

CiteScore

61.10

自引率

0.90%

发文量

审稿时长

2.1 months

期刊介绍： Science is a leading outlet for scientific news, commentary, and cutting-edge research. Through its print and online incarnations, Science reaches an estimated worldwide readership of more than one million. Science’s authorship is global too, and its articles consistently rank among the world's most cited research. Science serves as a forum for discussion of important issues related to the advancement of science by publishing material on which a consensus has been reached as well as including the presentation of minority or conflicting points of view. Accordingly, all articles published in Science—including editorials, news and comment, and book reviews—are signed and reflect the individual views of the authors and not official points of view adopted by AAAS or the institutions with which the authors are affiliated. Science seeks to publish those papers that are most influential in their fields or across fields and that will significantly advance scientific understanding. Selected papers should present novel and broadly important data, syntheses, or concepts. They should merit recognition by the wider scientific community and general public provided by publication in Science, beyond that provided by specialty journals. Science welcomes submissions from all fields of science and from any source. The editors are committed to the prompt evaluation and publication of submitted papers while upholding high standards that support reproducibility of published research. Science is published weekly; selected papers are published online ahead of print.