Kai Sun, Shiqi Geng, Jiaqian Yang, Faen Song, Yongqiang Gu, Haozhe Feng, Noritatsu Tsubaki, Qingde Zhang, Yisheng Tan
{"title":"以钾为媒介控制 CuCoAl 层状纳米板上吸附的中间产物,利用合成气合成乙醇","authors":"Kai Sun, Shiqi Geng, Jiaqian Yang, Faen Song, Yongqiang Gu, Haozhe Feng, Noritatsu Tsubaki, Qingde Zhang, Yisheng Tan","doi":"10.1016/j.fuel.2024.132404","DOIUrl":null,"url":null,"abstract":"A set of K-promoted CuCoAl nanoplates were synthesized via precipitation followed by impregnation method and assessed for syngas conversion. The optimized 1K-CuCo catalyst manifested a relatively higher total alcohols selectivity of 48.4 %, with ethanol comprising 35.4 % of total alcohols. As indicated by in situ CO DRIFT and XPS outcomes, on the 1K-CuCo catalyst surface, a distinct preference was observed for the adsorption of CO on Cu species (non-dissociative CO*) and bridging CO adsorption on Co species (dissociative CO*). A substantial presence of strongly adsorbed formate species, which contributed favorably to the production of CH* intermediates, was also identified on the optimal catalyst surface. More importantly, operando DRIFT characterization confirmed that K-modified CuCo catalyst effectively inhibited the hydrogenation (or coupling) of adsorbed CH* intermediates derived from formate species to generate methane and CH. Instead, the adsorbed CH* intermediates coupled with non-dissociated CO* to form CHCO* species. Therefore, the K promoter can finely regulate the adsorption strength and distribution of intermediates species, thus furnishing sufficient CH* intermediates and CO* species to take part in CH-CO coupling reaction to synthesize ethanol.","PeriodicalId":325,"journal":{"name":"Fuel","volume":null,"pages":null},"PeriodicalIF":6.7000,"publicationDate":"2024-07-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Potassium-mediated control of adsorbed intermediates on CuCoAl layered nanoplates for ethanol synthesis from syngas\",\"authors\":\"Kai Sun, Shiqi Geng, Jiaqian Yang, Faen Song, Yongqiang Gu, Haozhe Feng, Noritatsu Tsubaki, Qingde Zhang, Yisheng Tan\",\"doi\":\"10.1016/j.fuel.2024.132404\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"A set of K-promoted CuCoAl nanoplates were synthesized via precipitation followed by impregnation method and assessed for syngas conversion. The optimized 1K-CuCo catalyst manifested a relatively higher total alcohols selectivity of 48.4 %, with ethanol comprising 35.4 % of total alcohols. As indicated by in situ CO DRIFT and XPS outcomes, on the 1K-CuCo catalyst surface, a distinct preference was observed for the adsorption of CO on Cu species (non-dissociative CO*) and bridging CO adsorption on Co species (dissociative CO*). A substantial presence of strongly adsorbed formate species, which contributed favorably to the production of CH* intermediates, was also identified on the optimal catalyst surface. More importantly, operando DRIFT characterization confirmed that K-modified CuCo catalyst effectively inhibited the hydrogenation (or coupling) of adsorbed CH* intermediates derived from formate species to generate methane and CH. Instead, the adsorbed CH* intermediates coupled with non-dissociated CO* to form CHCO* species. Therefore, the K promoter can finely regulate the adsorption strength and distribution of intermediates species, thus furnishing sufficient CH* intermediates and CO* species to take part in CH-CO coupling reaction to synthesize ethanol.\",\"PeriodicalId\":325,\"journal\":{\"name\":\"Fuel\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":6.7000,\"publicationDate\":\"2024-07-04\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Fuel\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://doi.org/10.1016/j.fuel.2024.132404\",\"RegionNum\":1,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"ENERGY & FUELS\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Fuel","FirstCategoryId":"5","ListUrlMain":"https://doi.org/10.1016/j.fuel.2024.132404","RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"ENERGY & FUELS","Score":null,"Total":0}
Potassium-mediated control of adsorbed intermediates on CuCoAl layered nanoplates for ethanol synthesis from syngas
A set of K-promoted CuCoAl nanoplates were synthesized via precipitation followed by impregnation method and assessed for syngas conversion. The optimized 1K-CuCo catalyst manifested a relatively higher total alcohols selectivity of 48.4 %, with ethanol comprising 35.4 % of total alcohols. As indicated by in situ CO DRIFT and XPS outcomes, on the 1K-CuCo catalyst surface, a distinct preference was observed for the adsorption of CO on Cu species (non-dissociative CO*) and bridging CO adsorption on Co species (dissociative CO*). A substantial presence of strongly adsorbed formate species, which contributed favorably to the production of CH* intermediates, was also identified on the optimal catalyst surface. More importantly, operando DRIFT characterization confirmed that K-modified CuCo catalyst effectively inhibited the hydrogenation (or coupling) of adsorbed CH* intermediates derived from formate species to generate methane and CH. Instead, the adsorbed CH* intermediates coupled with non-dissociated CO* to form CHCO* species. Therefore, the K promoter can finely regulate the adsorption strength and distribution of intermediates species, thus furnishing sufficient CH* intermediates and CO* species to take part in CH-CO coupling reaction to synthesize ethanol.
期刊介绍:
The exploration of energy sources remains a critical matter of study. For the past nine decades, fuel has consistently held the forefront in primary research efforts within the field of energy science. This area of investigation encompasses a wide range of subjects, with a particular emphasis on emerging concerns like environmental factors and pollution.