Quantifying the Site Heterogeneities of Non-Uniform Catalysts Using QuantEXAFS

IF 6.1 Q1 CHEMISTRY, MULTIDISCIPLINARY
Rachita Rana, Jiyun Hong, Adam S. Hoffman, Baraa Werghi, Simon R. Bare, Ambarish R. Kulkarni
{"title":"Quantifying the Site Heterogeneities of Non-Uniform Catalysts Using QuantEXAFS","authors":"Rachita Rana,&nbsp;Jiyun Hong,&nbsp;Adam S. Hoffman,&nbsp;Baraa Werghi,&nbsp;Simon R. Bare,&nbsp;Ambarish R. Kulkarni","doi":"10.1002/cmtd.202400020","DOIUrl":null,"url":null,"abstract":"<p>We present the Multi-site (MS) QuantEXAFS approach, designed to model the EXAFS data from samples containing an element in different local bonding geometries. Building upon our QuantEXAFS method, which maps experimental extended X-ray absorption fine structures (EXAFS) data to DFT-optimized structures, MS-QuantEXAFS introduces the key capability to probe fractional contributions of multiple sites that may be present in an experimental sample. Specifically, we demonstrate effectiveness of this technique by investigating mixed samples containing known fractions of site-isolated subsurface Pt/MgO with Pt nanoparticles uniformly supported on MgO. The ‘site-fractions’ obtained through MS-QuantEXAFS closely match (i. e., ±6%) the known fractions of the physically mixed samples. This approach has been generalized to other oxides, and thus represents an important advance in quantifying the speciation of non-uniform catalyst samples.</p>","PeriodicalId":72562,"journal":{"name":"Chemistry methods : new approaches to solving problems in chemistry","volume":"5 1","pages":""},"PeriodicalIF":6.1000,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cmtd.202400020","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chemistry methods : new approaches to solving problems in chemistry","FirstCategoryId":"1085","ListUrlMain":"https://onlinelibrary.wiley.com/doi/10.1002/cmtd.202400020","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0

Abstract

We present the Multi-site (MS) QuantEXAFS approach, designed to model the EXAFS data from samples containing an element in different local bonding geometries. Building upon our QuantEXAFS method, which maps experimental extended X-ray absorption fine structures (EXAFS) data to DFT-optimized structures, MS-QuantEXAFS introduces the key capability to probe fractional contributions of multiple sites that may be present in an experimental sample. Specifically, we demonstrate effectiveness of this technique by investigating mixed samples containing known fractions of site-isolated subsurface Pt/MgO with Pt nanoparticles uniformly supported on MgO. The ‘site-fractions’ obtained through MS-QuantEXAFS closely match (i. e., ±6%) the known fractions of the physically mixed samples. This approach has been generalized to other oxides, and thus represents an important advance in quantifying the speciation of non-uniform catalyst samples.

Abstract Image

使用QuantEXAFS定量非均匀催化剂的位点非均质性
我们提出了多位点(MS) QuantEXAFS方法,旨在对含有不同局部键合几何形状元素的样品的EXAFS数据进行建模。基于我们的QuantEXAFS方法(将实验扩展x射线吸收精细结构(EXAFS)数据映射到dft优化结构),MS-QuantEXAFS引入了探测实验样品中可能存在的多个位点的分数贡献的关键功能。具体来说,我们通过研究含有已知位点分离的地下Pt/MgO和均匀负载在MgO上的Pt纳米颗粒的混合样品,证明了该技术的有效性。通过MS-QuantEXAFS获得的“位点分数”密切匹配(即;(±6%)物理混合样品的已知分数。这种方法已经推广到其他氧化物,因此代表了量化非均匀催化剂样品形态的重要进展。
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
CiteScore
7.30
自引率
0.00%
发文量
0
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
确定
请完成安全验证×
copy
已复制链接
快去分享给好友吧!
我知道了
右上角分享
点击右上角分享
0
联系我们:info@booksci.cn Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。 Copyright © 2023 布克学术 All rights reserved.
京ICP备2023020795号-1
ghs 京公网安备 11010802042870号
Book学术文献互助
Book学术文献互助群
群 号:481959085
Book学术官方微信