Band Structure Engineering and Orbital Orientation Control Constructing Dual Active Sites for Efficient Sulfur Redox Reaction

The kinetics difference among multistep electrochemical processes leads to the accumulation of soluble polysulfides and thus shuttle effect in lithium−sulfur (Li−S) batteries. While the interaction between catalysts and representative species has been reported, the root of the kinetics difference, i...

Ausführliche Beschreibung

Gespeichert in:
Bibliographische Detailangaben
Veröffentlicht in:Advanced materials (Weinheim) 2024-01, Vol.36 (2), p.e2309024-n/a
Hauptverfasser: Lao, Zhoujie, Han, Zhiyuan, Ma, Jiabin, Zhang, Mengtian, Wu, Xinru, Jia, Yeyang, Gao, Runhua, Zhu, Yanfei, Xiao, Xiao, Yu, Kuang, Zhou, Guangmin
Format: Artikel
Sprache:eng
Schlagworte:
Online-Zugang:Volltext
Tags: Tag hinzufügen
Keine Tags, Fügen Sie den ersten Tag hinzu!
container_end_page n/a
container_issue 2
container_start_page e2309024
container_title Advanced materials (Weinheim)
container_volume 36
creator Lao, Zhoujie
Han, Zhiyuan
Ma, Jiabin
Zhang, Mengtian
Wu, Xinru
Jia, Yeyang
Gao, Runhua
Zhu, Yanfei
Xiao, Xiao
Yu, Kuang
Zhou, Guangmin
description The kinetics difference among multistep electrochemical processes leads to the accumulation of soluble polysulfides and thus shuttle effect in lithium−sulfur (Li−S) batteries. While the interaction between catalysts and representative species has been reported, the root of the kinetics difference, interaction change among redox reactions, remains unclear, which significantly impedes the catalysts design for Li−S batteries. Here, this work deciphers the interaction change among electrocatalytic sulfur reactions, using tungsten disulfide (WS2) a model system to demonstrate the efficiency of modifying electrocatalytic selectivity via dual‐coordination design. Band structure engineering and orbital orientation control are combined to guide the design of WS2 with boron dopants and sulfur vacancies (B−WS2−x), accurately modulating interaction with lithium and sulfur sites in polysulfide species for relatively higher interaction with short‐chain polysulfides. The modified interaction trend is experimentally confirmed by distinguishing the kinetics of each electrochemical reaction step, indicating the effectiveness of the designed strategy. An Ah‐level pouch cell with B−WS2−x delivers a gravimetric energy density of up to 417.6 Wh kg−1 with a low electrolyte/sulfur ratio of 3.6 µL mg−1 and negative/positive ratio of 1.2. This work presents a dual‐coordination strategy for advancing evolutionarily catalytic activity, offering a rational strategy to develop effective catalysts for practical Li−S batteries. Interaction trend among redox reactions affect evolutionarily electrocatalytic activity. Using WS2 as an example, band structure engineering and orbital orientation control are combined to construct Li−S and S−B dual‐coordination, accurately modulating the interaction trend to accelerate the rate‐determined process. This work presents a dual‐coordination design for advancing evolutionarily catalytic activity, helping with effective catalyst design for practical Li−S batteries.
doi_str_mv 10.1002/adma.202309024
format Article
fullrecord <record><control><sourceid>proquest_cross</sourceid><recordid>TN_cdi_proquest_miscellaneous_2878709786</recordid><sourceformat>XML</sourceformat><sourcesystem>PC</sourcesystem><sourcerecordid>2912956228</sourcerecordid><originalsourceid>FETCH-LOGICAL-c4274-a7cdd9c7d980d4f0fcbea82baf57edcc6525aaaf903238e52cd6079d9e33d7833</originalsourceid><addsrcrecordid>eNqFkc1vFCEchomxsWv16tGQePEy29_AzADHdbt-JDVNXD0Tlo-GZhYqDGoP_d_LuLVNvPTCS8LzPiF5EXrTwrIFIKfK7NWSAKEggHTP0KLtSdt0IPrnaAGC9o0YOn6MXuZ8BQBigOEFOqaMd5xytkC3H1QweDuloqeSLN6ESx-sTT5c4vnlIu38pMaa3oZJTT4GvI5hSnGcM_8tzvBZqdSq3n9ZvPWTzdjFhDfOeT038baMriT8zZr4p55Kz6pX6MipMdvX93mCfnzcfF9_bs4vPn1Zr84b3RHWNYppY4RmRnAwnQOnd1ZxslOuZ9ZoPfSkV0o5AZRQbnuizQBMGGEpNYxTeoLeH7zXKf4sNk9y77O246iCjSVLwhlnIBgfKvruP_QqlhTq7yQRLRH9QAiv1PJA6RRzTtbJ6-T3Kt3IFuQ8jJyHkQ_D1MLbe23Z7a15wP8tUQFxAH770d48oZOrs6-rR_kdaA2b8w</addsrcrecordid><sourcetype>Aggregation Database</sourcetype><iscdi>true</iscdi><recordtype>article</recordtype><pqid>2912956228</pqid></control><display><type>article</type><title>Band Structure Engineering and Orbital Orientation Control Constructing Dual Active Sites for Efficient Sulfur Redox Reaction</title><source>Wiley Online Library</source><creator>Lao, Zhoujie ; Han, Zhiyuan ; Ma, Jiabin ; Zhang, Mengtian ; Wu, Xinru ; Jia, Yeyang ; Gao, Runhua ; Zhu, Yanfei ; Xiao, Xiao ; Yu, Kuang ; Zhou, Guangmin</creator><creatorcontrib>Lao, Zhoujie ; Han, Zhiyuan ; Ma, Jiabin ; Zhang, Mengtian ; Wu, Xinru ; Jia, Yeyang ; Gao, Runhua ; Zhu, Yanfei ; Xiao, Xiao ; Yu, Kuang ; Zhou, Guangmin</creatorcontrib><description>The kinetics difference among multistep electrochemical processes leads to the accumulation of soluble polysulfides and thus shuttle effect in lithium−sulfur (Li−S) batteries. While the interaction between catalysts and representative species has been reported, the root of the kinetics difference, interaction change among redox reactions, remains unclear, which significantly impedes the catalysts design for Li−S batteries. Here, this work deciphers the interaction change among electrocatalytic sulfur reactions, using tungsten disulfide (WS2) a model system to demonstrate the efficiency of modifying electrocatalytic selectivity via dual‐coordination design. Band structure engineering and orbital orientation control are combined to guide the design of WS2 with boron dopants and sulfur vacancies (B−WS2−x), accurately modulating interaction with lithium and sulfur sites in polysulfide species for relatively higher interaction with short‐chain polysulfides. The modified interaction trend is experimentally confirmed by distinguishing the kinetics of each electrochemical reaction step, indicating the effectiveness of the designed strategy. An Ah‐level pouch cell with B−WS2−x delivers a gravimetric energy density of up to 417.6 Wh kg−1 with a low electrolyte/sulfur ratio of 3.6 µL mg−1 and negative/positive ratio of 1.2. This work presents a dual‐coordination strategy for advancing evolutionarily catalytic activity, offering a rational strategy to develop effective catalysts for practical Li−S batteries. Interaction trend among redox reactions affect evolutionarily electrocatalytic activity. Using WS2 as an example, band structure engineering and orbital orientation control are combined to construct Li−S and S−B dual‐coordination, accurately modulating the interaction trend to accelerate the rate‐determined process. This work presents a dual‐coordination design for advancing evolutionarily catalytic activity, helping with effective catalyst design for practical Li−S batteries.</description><identifier>ISSN: 0935-9648</identifier><identifier>EISSN: 1521-4095</identifier><identifier>DOI: 10.1002/adma.202309024</identifier><identifier>PMID: 37848387</identifier><language>eng</language><publisher>Germany: Wiley Subscription Services, Inc</publisher><subject>Active control ; band engineering ; Band structure of solids ; Catalysts ; Catalytic activity ; Coordination ; defect engineering ; dual‐coordination ; Kinetics ; Lithium ; Lithium sulfur batteries ; lithium–sulfur battery ; Polysulfides ; Redox reactions ; Sulfur ; sulfur redox reaction ; Tungsten disulfide</subject><ispartof>Advanced materials (Weinheim), 2024-01, Vol.36 (2), p.e2309024-n/a</ispartof><rights>2023 Wiley‐VCH GmbH</rights><rights>2023 Wiley-VCH GmbH.</rights><rights>2024 Wiley‐VCH GmbH</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c4274-a7cdd9c7d980d4f0fcbea82baf57edcc6525aaaf903238e52cd6079d9e33d7833</citedby><cites>FETCH-LOGICAL-c4274-a7cdd9c7d980d4f0fcbea82baf57edcc6525aaaf903238e52cd6079d9e33d7833</cites><orcidid>0000-0002-3629-5686</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://onlinelibrary.wiley.com/doi/pdf/10.1002%2Fadma.202309024$$EPDF$$P50$$Gwiley$$H</linktopdf><linktohtml>$$Uhttps://onlinelibrary.wiley.com/doi/full/10.1002%2Fadma.202309024$$EHTML$$P50$$Gwiley$$H</linktohtml><link.rule.ids>314,780,784,1417,27924,27925,45574,45575</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/37848387$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>Lao, Zhoujie</creatorcontrib><creatorcontrib>Han, Zhiyuan</creatorcontrib><creatorcontrib>Ma, Jiabin</creatorcontrib><creatorcontrib>Zhang, Mengtian</creatorcontrib><creatorcontrib>Wu, Xinru</creatorcontrib><creatorcontrib>Jia, Yeyang</creatorcontrib><creatorcontrib>Gao, Runhua</creatorcontrib><creatorcontrib>Zhu, Yanfei</creatorcontrib><creatorcontrib>Xiao, Xiao</creatorcontrib><creatorcontrib>Yu, Kuang</creatorcontrib><creatorcontrib>Zhou, Guangmin</creatorcontrib><title>Band Structure Engineering and Orbital Orientation Control Constructing Dual Active Sites for Efficient Sulfur Redox Reaction</title><title>Advanced materials (Weinheim)</title><addtitle>Adv Mater</addtitle><description>The kinetics difference among multistep electrochemical processes leads to the accumulation of soluble polysulfides and thus shuttle effect in lithium−sulfur (Li−S) batteries. While the interaction between catalysts and representative species has been reported, the root of the kinetics difference, interaction change among redox reactions, remains unclear, which significantly impedes the catalysts design for Li−S batteries. Here, this work deciphers the interaction change among electrocatalytic sulfur reactions, using tungsten disulfide (WS2) a model system to demonstrate the efficiency of modifying electrocatalytic selectivity via dual‐coordination design. Band structure engineering and orbital orientation control are combined to guide the design of WS2 with boron dopants and sulfur vacancies (B−WS2−x), accurately modulating interaction with lithium and sulfur sites in polysulfide species for relatively higher interaction with short‐chain polysulfides. The modified interaction trend is experimentally confirmed by distinguishing the kinetics of each electrochemical reaction step, indicating the effectiveness of the designed strategy. An Ah‐level pouch cell with B−WS2−x delivers a gravimetric energy density of up to 417.6 Wh kg−1 with a low electrolyte/sulfur ratio of 3.6 µL mg−1 and negative/positive ratio of 1.2. This work presents a dual‐coordination strategy for advancing evolutionarily catalytic activity, offering a rational strategy to develop effective catalysts for practical Li−S batteries. Interaction trend among redox reactions affect evolutionarily electrocatalytic activity. Using WS2 as an example, band structure engineering and orbital orientation control are combined to construct Li−S and S−B dual‐coordination, accurately modulating the interaction trend to accelerate the rate‐determined process. This work presents a dual‐coordination design for advancing evolutionarily catalytic activity, helping with effective catalyst design for practical Li−S batteries.</description><subject>Active control</subject><subject>band engineering</subject><subject>Band structure of solids</subject><subject>Catalysts</subject><subject>Catalytic activity</subject><subject>Coordination</subject><subject>defect engineering</subject><subject>dual‐coordination</subject><subject>Kinetics</subject><subject>Lithium</subject><subject>Lithium sulfur batteries</subject><subject>lithium–sulfur battery</subject><subject>Polysulfides</subject><subject>Redox reactions</subject><subject>Sulfur</subject><subject>sulfur redox reaction</subject><subject>Tungsten disulfide</subject><issn>0935-9648</issn><issn>1521-4095</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2024</creationdate><recordtype>article</recordtype><recordid>eNqFkc1vFCEchomxsWv16tGQePEy29_AzADHdbt-JDVNXD0Tlo-GZhYqDGoP_d_LuLVNvPTCS8LzPiF5EXrTwrIFIKfK7NWSAKEggHTP0KLtSdt0IPrnaAGC9o0YOn6MXuZ8BQBigOEFOqaMd5xytkC3H1QweDuloqeSLN6ESx-sTT5c4vnlIu38pMaa3oZJTT4GvI5hSnGcM_8tzvBZqdSq3n9ZvPWTzdjFhDfOeT038baMriT8zZr4p55Kz6pX6MipMdvX93mCfnzcfF9_bs4vPn1Zr84b3RHWNYppY4RmRnAwnQOnd1ZxslOuZ9ZoPfSkV0o5AZRQbnuizQBMGGEpNYxTeoLeH7zXKf4sNk9y77O246iCjSVLwhlnIBgfKvruP_QqlhTq7yQRLRH9QAiv1PJA6RRzTtbJ6-T3Kt3IFuQ8jJyHkQ_D1MLbe23Z7a15wP8tUQFxAH770d48oZOrs6-rR_kdaA2b8w</recordid><startdate>20240101</startdate><enddate>20240101</enddate><creator>Lao, Zhoujie</creator><creator>Han, Zhiyuan</creator><creator>Ma, Jiabin</creator><creator>Zhang, Mengtian</creator><creator>Wu, Xinru</creator><creator>Jia, Yeyang</creator><creator>Gao, Runhua</creator><creator>Zhu, Yanfei</creator><creator>Xiao, Xiao</creator><creator>Yu, Kuang</creator><creator>Zhou, Guangmin</creator><general>Wiley Subscription Services, Inc</general><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7SR</scope><scope>8BQ</scope><scope>8FD</scope><scope>JG9</scope><scope>7X8</scope><orcidid>https://orcid.org/0000-0002-3629-5686</orcidid></search><sort><creationdate>20240101</creationdate><title>Band Structure Engineering and Orbital Orientation Control Constructing Dual Active Sites for Efficient Sulfur Redox Reaction</title><author>Lao, Zhoujie ; Han, Zhiyuan ; Ma, Jiabin ; Zhang, Mengtian ; Wu, Xinru ; Jia, Yeyang ; Gao, Runhua ; Zhu, Yanfei ; Xiao, Xiao ; Yu, Kuang ; Zhou, Guangmin</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c4274-a7cdd9c7d980d4f0fcbea82baf57edcc6525aaaf903238e52cd6079d9e33d7833</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2024</creationdate><topic>Active control</topic><topic>band engineering</topic><topic>Band structure of solids</topic><topic>Catalysts</topic><topic>Catalytic activity</topic><topic>Coordination</topic><topic>defect engineering</topic><topic>dual‐coordination</topic><topic>Kinetics</topic><topic>Lithium</topic><topic>Lithium sulfur batteries</topic><topic>lithium–sulfur battery</topic><topic>Polysulfides</topic><topic>Redox reactions</topic><topic>Sulfur</topic><topic>sulfur redox reaction</topic><topic>Tungsten disulfide</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Lao, Zhoujie</creatorcontrib><creatorcontrib>Han, Zhiyuan</creatorcontrib><creatorcontrib>Ma, Jiabin</creatorcontrib><creatorcontrib>Zhang, Mengtian</creatorcontrib><creatorcontrib>Wu, Xinru</creatorcontrib><creatorcontrib>Jia, Yeyang</creatorcontrib><creatorcontrib>Gao, Runhua</creatorcontrib><creatorcontrib>Zhu, Yanfei</creatorcontrib><creatorcontrib>Xiao, Xiao</creatorcontrib><creatorcontrib>Yu, Kuang</creatorcontrib><creatorcontrib>Zhou, Guangmin</creatorcontrib><collection>PubMed</collection><collection>CrossRef</collection><collection>Engineered Materials Abstracts</collection><collection>METADEX</collection><collection>Technology Research Database</collection><collection>Materials Research Database</collection><collection>MEDLINE - Academic</collection><jtitle>Advanced materials (Weinheim)</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Lao, Zhoujie</au><au>Han, Zhiyuan</au><au>Ma, Jiabin</au><au>Zhang, Mengtian</au><au>Wu, Xinru</au><au>Jia, Yeyang</au><au>Gao, Runhua</au><au>Zhu, Yanfei</au><au>Xiao, Xiao</au><au>Yu, Kuang</au><au>Zhou, Guangmin</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Band Structure Engineering and Orbital Orientation Control Constructing Dual Active Sites for Efficient Sulfur Redox Reaction</atitle><jtitle>Advanced materials (Weinheim)</jtitle><addtitle>Adv Mater</addtitle><date>2024-01-01</date><risdate>2024</risdate><volume>36</volume><issue>2</issue><spage>e2309024</spage><epage>n/a</epage><pages>e2309024-n/a</pages><issn>0935-9648</issn><eissn>1521-4095</eissn><abstract>The kinetics difference among multistep electrochemical processes leads to the accumulation of soluble polysulfides and thus shuttle effect in lithium−sulfur (Li−S) batteries. While the interaction between catalysts and representative species has been reported, the root of the kinetics difference, interaction change among redox reactions, remains unclear, which significantly impedes the catalysts design for Li−S batteries. Here, this work deciphers the interaction change among electrocatalytic sulfur reactions, using tungsten disulfide (WS2) a model system to demonstrate the efficiency of modifying electrocatalytic selectivity via dual‐coordination design. Band structure engineering and orbital orientation control are combined to guide the design of WS2 with boron dopants and sulfur vacancies (B−WS2−x), accurately modulating interaction with lithium and sulfur sites in polysulfide species for relatively higher interaction with short‐chain polysulfides. The modified interaction trend is experimentally confirmed by distinguishing the kinetics of each electrochemical reaction step, indicating the effectiveness of the designed strategy. An Ah‐level pouch cell with B−WS2−x delivers a gravimetric energy density of up to 417.6 Wh kg−1 with a low electrolyte/sulfur ratio of 3.6 µL mg−1 and negative/positive ratio of 1.2. This work presents a dual‐coordination strategy for advancing evolutionarily catalytic activity, offering a rational strategy to develop effective catalysts for practical Li−S batteries. Interaction trend among redox reactions affect evolutionarily electrocatalytic activity. Using WS2 as an example, band structure engineering and orbital orientation control are combined to construct Li−S and S−B dual‐coordination, accurately modulating the interaction trend to accelerate the rate‐determined process. This work presents a dual‐coordination design for advancing evolutionarily catalytic activity, helping with effective catalyst design for practical Li−S batteries.</abstract><cop>Germany</cop><pub>Wiley Subscription Services, Inc</pub><pmid>37848387</pmid><doi>10.1002/adma.202309024</doi><tpages>11</tpages><orcidid>https://orcid.org/0000-0002-3629-5686</orcidid></addata></record>
fulltext fulltext
identifier ISSN: 0935-9648
ispartof Advanced materials (Weinheim), 2024-01, Vol.36 (2), p.e2309024-n/a
issn 0935-9648
1521-4095
language eng
recordid cdi_proquest_miscellaneous_2878709786
source Wiley Online Library
subjects Active control
band engineering
Band structure of solids
Catalysts
Catalytic activity
Coordination
defect engineering
dual‐coordination
Kinetics
Lithium
Lithium sulfur batteries
lithium–sulfur battery
Polysulfides
Redox reactions
Sulfur
sulfur redox reaction
Tungsten disulfide
title Band Structure Engineering and Orbital Orientation Control Constructing Dual Active Sites for Efficient Sulfur Redox Reaction
url https://sfx.bib-bvb.de/sfx_tum?ctx_ver=Z39.88-2004&ctx_enc=info:ofi/enc:UTF-8&ctx_tim=2024-12-25T11%3A45%3A39IST&url_ver=Z39.88-2004&url_ctx_fmt=infofi/fmt:kev:mtx:ctx&rfr_id=info:sid/primo.exlibrisgroup.com:primo3-Article-proquest_cross&rft_val_fmt=info:ofi/fmt:kev:mtx:journal&rft.genre=article&rft.atitle=Band%20Structure%20Engineering%20and%20Orbital%20Orientation%20Control%20Constructing%20Dual%20Active%20Sites%20for%20Efficient%20Sulfur%20Redox%20Reaction&rft.jtitle=Advanced%20materials%20(Weinheim)&rft.au=Lao,%20Zhoujie&rft.date=2024-01-01&rft.volume=36&rft.issue=2&rft.spage=e2309024&rft.epage=n/a&rft.pages=e2309024-n/a&rft.issn=0935-9648&rft.eissn=1521-4095&rft_id=info:doi/10.1002/adma.202309024&rft_dat=%3Cproquest_cross%3E2912956228%3C/proquest_cross%3E%3Curl%3E%3C/url%3E&disable_directlink=true&sfx.directlink=off&sfx.report_link=0&rft_id=info:oai/&rft_pqid=2912956228&rft_id=info:pmid/37848387&rfr_iscdi=true