Loading…

Enhanced metal-support interaction between Pd and hierarchical NbO oxygen defect induction to promote CO oxidative coupling to dimethyl oxalate

Production of ethylene glycol from coal is a particularly interesting route as it is an economic alternative to the petrochemical-based route. In this process, effectively generating dimethyl oxalate (DMO) is a crucial step by CO oxidative coupling reaction under Pd-based catalysts. However, the agg...

Full description

Saved in:
Bibliographic Details
Published in:Nanoscale 2021-11, Vol.13 (44), p.18773-18779
Main Authors: Tan, Hongzi, Xu, Yu-Ping, Rong, Siteng, Zhao, Rongrong, Cui, Hongyou, Chen, Zhe-Ning, Xu, Zhong-Ning, Zhang, Ning-Ning, Guo, Guo-Cong
Format: Article
Language:
Online Access:Get full text
Tags: Add Tag
No Tags, Be the first to tag this record!
cited_by
cites
container_end_page 18779
container_issue 44
container_start_page 18773
container_title Nanoscale
container_volume 13
creator Tan, Hongzi
Xu, Yu-Ping
Rong, Siteng
Zhao, Rongrong
Cui, Hongyou
Chen, Zhe-Ning
Xu, Zhong-Ning
Zhang, Ning-Ning
Guo, Guo-Cong
description Production of ethylene glycol from coal is a particularly interesting route as it is an economic alternative to the petrochemical-based route. In this process, effectively generating dimethyl oxalate (DMO) is a crucial step by CO oxidative coupling reaction under Pd-based catalysts. However, the aggregation of Pd species over the support is still an issue that relates to the deterioration of catalytic activity and stability. To this end, enhancing the metal-support interaction is urgently required. In this work, hierarchical Nb 2 O 5 (H-Nb 2 O 5 ) microspheres with abundant oxygen defects were synthesized to anchor the Pd species thus promoting the electron transfer between Pd species and Nb species associated with the generation of interfacial Pd-NbO x sites. Besides, the thinned electron density of Pd species resulting from the electron-withdrawing effect of Nb species is beneficial for activating the adsorbed CO molecules, leading to superior catalytic activity. The Pd/H-Nb 2 O 5 catalyst exhibited 63.1% of CO conversion (theoretical maximum conversion: 64.3%) and 92.9% of DMO selectivity, with a DMO weight time yield of 1297.9 g kg cat. −1 h −1 , and remained robust even after 50 h of time on stream evaluation. Current work provides a deep insight into the CO activation mechanism and helps improve the catalytic stability by boosting interfacial electron interaction via oxygen defects induction, and also sheds light on the design and synthesis of high-performance catalysts in other heterogeneous catalysis fields. Production of ethylene glycol from coal is a particularly interesting route as it is an economic alternative to the petrochemical-based route.
doi_str_mv 10.1039/d1nr03370k
format article
fullrecord <record><control><sourceid>rsc</sourceid><recordid>TN_cdi_rsc_primary_d1nr03370k</recordid><sourceformat>XML</sourceformat><sourcesystem>PC</sourcesystem><sourcerecordid>d1nr03370k</sourcerecordid><originalsourceid>FETCH-rsc_primary_d1nr03370k3</originalsourceid><addsrcrecordid>eNqFj71OAzEQhC0EEuGnoY-0L3DEF0eHUkdBVECRPtrYm5zBZ1v2XuCeglfGJxCUqXZW34xGI8RdLe9rqZYzU_sklXqQ72diMpcLWZVnfv6nm8WluMr5TcpmqRo1EV9r36LXZKAjRlflPsaQGKxnSqjZBg874g8iD68G0BtobSFJt1ajg-fdC4TP4VCwoT3pMWn6nxwHiCl0gQlWo8saZHsk0KGPzvrDaDC29LaDKxgdMt2Iiz26TLe_91pMH9eb1VOVst7GZDtMw_Z_pTrFvwHSSVkW</addsrcrecordid><sourcetype>Publisher</sourcetype><iscdi>true</iscdi><recordtype>article</recordtype></control><display><type>article</type><title>Enhanced metal-support interaction between Pd and hierarchical NbO oxygen defect induction to promote CO oxidative coupling to dimethyl oxalate</title><source>Royal Society of Chemistry:Jisc Collections:Royal Society of Chemistry Read and Publish 2022-2024 (reading list)</source><creator>Tan, Hongzi ; Xu, Yu-Ping ; Rong, Siteng ; Zhao, Rongrong ; Cui, Hongyou ; Chen, Zhe-Ning ; Xu, Zhong-Ning ; Zhang, Ning-Ning ; Guo, Guo-Cong</creator><creatorcontrib>Tan, Hongzi ; Xu, Yu-Ping ; Rong, Siteng ; Zhao, Rongrong ; Cui, Hongyou ; Chen, Zhe-Ning ; Xu, Zhong-Ning ; Zhang, Ning-Ning ; Guo, Guo-Cong</creatorcontrib><description>Production of ethylene glycol from coal is a particularly interesting route as it is an economic alternative to the petrochemical-based route. In this process, effectively generating dimethyl oxalate (DMO) is a crucial step by CO oxidative coupling reaction under Pd-based catalysts. However, the aggregation of Pd species over the support is still an issue that relates to the deterioration of catalytic activity and stability. To this end, enhancing the metal-support interaction is urgently required. In this work, hierarchical Nb 2 O 5 (H-Nb 2 O 5 ) microspheres with abundant oxygen defects were synthesized to anchor the Pd species thus promoting the electron transfer between Pd species and Nb species associated with the generation of interfacial Pd-NbO x sites. Besides, the thinned electron density of Pd species resulting from the electron-withdrawing effect of Nb species is beneficial for activating the adsorbed CO molecules, leading to superior catalytic activity. The Pd/H-Nb 2 O 5 catalyst exhibited 63.1% of CO conversion (theoretical maximum conversion: 64.3%) and 92.9% of DMO selectivity, with a DMO weight time yield of 1297.9 g kg cat. −1 h −1 , and remained robust even after 50 h of time on stream evaluation. Current work provides a deep insight into the CO activation mechanism and helps improve the catalytic stability by boosting interfacial electron interaction via oxygen defects induction, and also sheds light on the design and synthesis of high-performance catalysts in other heterogeneous catalysis fields. Production of ethylene glycol from coal is a particularly interesting route as it is an economic alternative to the petrochemical-based route.</description><identifier>ISSN: 2040-3364</identifier><identifier>EISSN: 2040-3372</identifier><identifier>DOI: 10.1039/d1nr03370k</identifier><ispartof>Nanoscale, 2021-11, Vol.13 (44), p.18773-18779</ispartof><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>314,780,784,27924,27925</link.rule.ids></links><search><creatorcontrib>Tan, Hongzi</creatorcontrib><creatorcontrib>Xu, Yu-Ping</creatorcontrib><creatorcontrib>Rong, Siteng</creatorcontrib><creatorcontrib>Zhao, Rongrong</creatorcontrib><creatorcontrib>Cui, Hongyou</creatorcontrib><creatorcontrib>Chen, Zhe-Ning</creatorcontrib><creatorcontrib>Xu, Zhong-Ning</creatorcontrib><creatorcontrib>Zhang, Ning-Ning</creatorcontrib><creatorcontrib>Guo, Guo-Cong</creatorcontrib><title>Enhanced metal-support interaction between Pd and hierarchical NbO oxygen defect induction to promote CO oxidative coupling to dimethyl oxalate</title><title>Nanoscale</title><description>Production of ethylene glycol from coal is a particularly interesting route as it is an economic alternative to the petrochemical-based route. In this process, effectively generating dimethyl oxalate (DMO) is a crucial step by CO oxidative coupling reaction under Pd-based catalysts. However, the aggregation of Pd species over the support is still an issue that relates to the deterioration of catalytic activity and stability. To this end, enhancing the metal-support interaction is urgently required. In this work, hierarchical Nb 2 O 5 (H-Nb 2 O 5 ) microspheres with abundant oxygen defects were synthesized to anchor the Pd species thus promoting the electron transfer between Pd species and Nb species associated with the generation of interfacial Pd-NbO x sites. Besides, the thinned electron density of Pd species resulting from the electron-withdrawing effect of Nb species is beneficial for activating the adsorbed CO molecules, leading to superior catalytic activity. The Pd/H-Nb 2 O 5 catalyst exhibited 63.1% of CO conversion (theoretical maximum conversion: 64.3%) and 92.9% of DMO selectivity, with a DMO weight time yield of 1297.9 g kg cat. −1 h −1 , and remained robust even after 50 h of time on stream evaluation. Current work provides a deep insight into the CO activation mechanism and helps improve the catalytic stability by boosting interfacial electron interaction via oxygen defects induction, and also sheds light on the design and synthesis of high-performance catalysts in other heterogeneous catalysis fields. Production of ethylene glycol from coal is a particularly interesting route as it is an economic alternative to the petrochemical-based route.</description><issn>2040-3364</issn><issn>2040-3372</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2021</creationdate><recordtype>article</recordtype><sourceid/><recordid>eNqFj71OAzEQhC0EEuGnoY-0L3DEF0eHUkdBVECRPtrYm5zBZ1v2XuCeglfGJxCUqXZW34xGI8RdLe9rqZYzU_sklXqQ72diMpcLWZVnfv6nm8WluMr5TcpmqRo1EV9r36LXZKAjRlflPsaQGKxnSqjZBg874g8iD68G0BtobSFJt1ajg-fdC4TP4VCwoT3pMWn6nxwHiCl0gQlWo8saZHsk0KGPzvrDaDC29LaDKxgdMt2Iiz26TLe_91pMH9eb1VOVst7GZDtMw_Z_pTrFvwHSSVkW</recordid><startdate>20211118</startdate><enddate>20211118</enddate><creator>Tan, Hongzi</creator><creator>Xu, Yu-Ping</creator><creator>Rong, Siteng</creator><creator>Zhao, Rongrong</creator><creator>Cui, Hongyou</creator><creator>Chen, Zhe-Ning</creator><creator>Xu, Zhong-Ning</creator><creator>Zhang, Ning-Ning</creator><creator>Guo, Guo-Cong</creator><scope/></search><sort><creationdate>20211118</creationdate><title>Enhanced metal-support interaction between Pd and hierarchical NbO oxygen defect induction to promote CO oxidative coupling to dimethyl oxalate</title><author>Tan, Hongzi ; Xu, Yu-Ping ; Rong, Siteng ; Zhao, Rongrong ; Cui, Hongyou ; Chen, Zhe-Ning ; Xu, Zhong-Ning ; Zhang, Ning-Ning ; Guo, Guo-Cong</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-rsc_primary_d1nr03370k3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><creationdate>2021</creationdate><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Tan, Hongzi</creatorcontrib><creatorcontrib>Xu, Yu-Ping</creatorcontrib><creatorcontrib>Rong, Siteng</creatorcontrib><creatorcontrib>Zhao, Rongrong</creatorcontrib><creatorcontrib>Cui, Hongyou</creatorcontrib><creatorcontrib>Chen, Zhe-Ning</creatorcontrib><creatorcontrib>Xu, Zhong-Ning</creatorcontrib><creatorcontrib>Zhang, Ning-Ning</creatorcontrib><creatorcontrib>Guo, Guo-Cong</creatorcontrib><jtitle>Nanoscale</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Tan, Hongzi</au><au>Xu, Yu-Ping</au><au>Rong, Siteng</au><au>Zhao, Rongrong</au><au>Cui, Hongyou</au><au>Chen, Zhe-Ning</au><au>Xu, Zhong-Ning</au><au>Zhang, Ning-Ning</au><au>Guo, Guo-Cong</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Enhanced metal-support interaction between Pd and hierarchical NbO oxygen defect induction to promote CO oxidative coupling to dimethyl oxalate</atitle><jtitle>Nanoscale</jtitle><date>2021-11-18</date><risdate>2021</risdate><volume>13</volume><issue>44</issue><spage>18773</spage><epage>18779</epage><pages>18773-18779</pages><issn>2040-3364</issn><eissn>2040-3372</eissn><abstract>Production of ethylene glycol from coal is a particularly interesting route as it is an economic alternative to the petrochemical-based route. In this process, effectively generating dimethyl oxalate (DMO) is a crucial step by CO oxidative coupling reaction under Pd-based catalysts. However, the aggregation of Pd species over the support is still an issue that relates to the deterioration of catalytic activity and stability. To this end, enhancing the metal-support interaction is urgently required. In this work, hierarchical Nb 2 O 5 (H-Nb 2 O 5 ) microspheres with abundant oxygen defects were synthesized to anchor the Pd species thus promoting the electron transfer between Pd species and Nb species associated with the generation of interfacial Pd-NbO x sites. Besides, the thinned electron density of Pd species resulting from the electron-withdrawing effect of Nb species is beneficial for activating the adsorbed CO molecules, leading to superior catalytic activity. The Pd/H-Nb 2 O 5 catalyst exhibited 63.1% of CO conversion (theoretical maximum conversion: 64.3%) and 92.9% of DMO selectivity, with a DMO weight time yield of 1297.9 g kg cat. −1 h −1 , and remained robust even after 50 h of time on stream evaluation. Current work provides a deep insight into the CO activation mechanism and helps improve the catalytic stability by boosting interfacial electron interaction via oxygen defects induction, and also sheds light on the design and synthesis of high-performance catalysts in other heterogeneous catalysis fields. Production of ethylene glycol from coal is a particularly interesting route as it is an economic alternative to the petrochemical-based route.</abstract><doi>10.1039/d1nr03370k</doi><tpages>7</tpages></addata></record>
fulltext fulltext
identifier ISSN: 2040-3364
ispartof Nanoscale, 2021-11, Vol.13 (44), p.18773-18779
issn 2040-3364
2040-3372
language
recordid cdi_rsc_primary_d1nr03370k
source Royal Society of Chemistry:Jisc Collections:Royal Society of Chemistry Read and Publish 2022-2024 (reading list)
title Enhanced metal-support interaction between Pd and hierarchical NbO oxygen defect induction to promote CO oxidative coupling to dimethyl oxalate
url http://sfxeu10.hosted.exlibrisgroup.com/loughborough?ctx_ver=Z39.88-2004&ctx_enc=info:ofi/enc:UTF-8&ctx_tim=2024-12-18T15%3A48%3A10IST&url_ver=Z39.88-2004&url_ctx_fmt=infofi/fmt:kev:mtx:ctx&rfr_id=info:sid/primo.exlibrisgroup.com:primo3-Article-rsc&rft_val_fmt=info:ofi/fmt:kev:mtx:journal&rft.genre=article&rft.atitle=Enhanced%20metal-support%20interaction%20between%20Pd%20and%20hierarchical%20NbO%20oxygen%20defect%20induction%20to%20promote%20CO%20oxidative%20coupling%20to%20dimethyl%20oxalate&rft.jtitle=Nanoscale&rft.au=Tan,%20Hongzi&rft.date=2021-11-18&rft.volume=13&rft.issue=44&rft.spage=18773&rft.epage=18779&rft.pages=18773-18779&rft.issn=2040-3364&rft.eissn=2040-3372&rft_id=info:doi/10.1039/d1nr03370k&rft_dat=%3Crsc%3Ed1nr03370k%3C/rsc%3E%3Cgrp_id%3Ecdi_FETCH-rsc_primary_d1nr03370k3%3C/grp_id%3E%3Coa%3E%3C/oa%3E%3Curl%3E%3C/url%3E&rft_id=info:oai/&rft_id=info:pmid/&rfr_iscdi=true