Pub Date : 2024-11-21DOI: 10.1016/j.cclet.2024.110616
Chu Chu, Yuancheng Qin, Cailing Ni, Jianping Zou
{"title":"Corrigendum to “Halogenated benzothiadiazole-based conjugated polymers as efficient photocatalysts for dye degradation and oxidative coupling of benzylamines” [Chinese Chemical Letters 33 (2022) 2736–2740]","authors":"Chu Chu, Yuancheng Qin, Cailing Ni, Jianping Zou","doi":"10.1016/j.cclet.2024.110616","DOIUrl":"10.1016/j.cclet.2024.110616","url":null,"abstract":"","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 2","pages":"Article 110616"},"PeriodicalIF":9.4,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142699590","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-16DOI: 10.1016/j.cclet.2024.110545
Xue Zheng , Jizhen Xie , Xing Zhang , Weiting Sun , Heyang Zhao , Yantuan Li , Cheng Wang
{"title":"Corrigendum to “An overview of polymeric nanomicelles in clinical trials and on the market” [Chinese Chemical Letters 32 (2021) 243-257]","authors":"Xue Zheng , Jizhen Xie , Xing Zhang , Weiting Sun , Heyang Zhao , Yantuan Li , Cheng Wang","doi":"10.1016/j.cclet.2024.110545","DOIUrl":"10.1016/j.cclet.2024.110545","url":null,"abstract":"","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 2","pages":"Article 110545"},"PeriodicalIF":9.4,"publicationDate":"2024-11-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142650838","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-16DOI: 10.1016/j.cclet.2024.110562
Hui Liu , Xi Xiang , Jian-Bo Huang , Bi-Hui Zhu , Li-Yun Wang , Yuan-Jiao Tang , Fang-Xue Du , Ling Li , Feng Yan , Lang Ma , Li Qiu
{"title":"Corrigendum to “Ultrasound augmenting injectable chemotaxis hydrogel for articular cartilage repair in osteoarthritis” [Chinese Chemical Letters 32 (2021) 1759-1764]","authors":"Hui Liu , Xi Xiang , Jian-Bo Huang , Bi-Hui Zhu , Li-Yun Wang , Yuan-Jiao Tang , Fang-Xue Du , Ling Li , Feng Yan , Lang Ma , Li Qiu","doi":"10.1016/j.cclet.2024.110562","DOIUrl":"10.1016/j.cclet.2024.110562","url":null,"abstract":"","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 2","pages":"Article 110562"},"PeriodicalIF":9.4,"publicationDate":"2024-11-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142657004","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-06DOI: 10.1016/j.cclet.2024.109934
Jia-Ru Li , Ning Li , Li-Ling He , Jun He
Zirconium-based metal-organic cages (Zr-MOCs) typically exhibit high stability, but their structural and application reports are scarce due to stringent crystallization conditions. We have successfully fluorinated the classical Zr-MOCs (ZrT-3) for the first time, obtaining the fluorinated MOCs (ZrT-3-F). Notably, ZrT-3-F not only inherits the high stability of its parent structure, but also acts as a catalyst for the effective oxidation of benzyl thioether for the first time. The reaction can reach a conversion rate of 99 % in 6 h, and the selectivity reaches 95 %, which far exceeds the non-fluorinated ZrT-3. This work proves that the specific functionalization of the classical Zr-MOCs can further expand their application potential, such as catalysis.
{"title":"Fluorine-functionalized zirconium-organic cages for efficient photocatalytic oxidation of thioanisole","authors":"Jia-Ru Li , Ning Li , Li-Ling He , Jun He","doi":"10.1016/j.cclet.2024.109934","DOIUrl":"10.1016/j.cclet.2024.109934","url":null,"abstract":"<div><div>Zirconium-based metal-organic cages (Zr-MOCs) typically exhibit high stability, but their structural and application reports are scarce due to stringent crystallization conditions. We have successfully fluorinated the classical Zr-MOCs (<strong>ZrT-3</strong>) for the first time, obtaining the fluorinated MOCs (<strong>ZrT-3-F</strong>). Notably, <strong>ZrT-3-F</strong> not only inherits the high stability of its parent structure, but also acts as a catalyst for the effective oxidation of benzyl thioether for the first time. The reaction can reach a conversion rate of 99 % in 6 h, and the selectivity reaches 95 %, which far exceeds the non-fluorinated <strong>ZrT-3</strong>. This work proves that the specific functionalization of the classical Zr-MOCs can further expand their application potential, such as catalysis.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 1","pages":"Article 109934"},"PeriodicalIF":9.4,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142592883","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-05DOI: 10.1016/j.cclet.2024.110612
Qing Li , Yumei Feng , Yingjie Yu , Yazhou Chen , Yuhua Xie , Fang Luo , Zehui Yang
Efficient and stable electrocatalyst for oxygen evolution reaction (OER) in acidic environment is vital for polymer electrolyte membrane water electrolysis (PEMWE). In this work, we have devised the formation of heterostructured RuO2/MnO2 with nanoflower structure for acidic OER catalysis. Compared to commercial RuO2, the overpotential at 50 mA/cm2 is decreased by 36 mV, corresponding to a 3.7-fold better mass activity. The boosted acidic OER performance is attributed to the heterostructure inducing more electrons are filled in eg orbital of Ru atom triggering a better deprotonation of bridge oxygen atom in Ru-Obri-Mn structure evidenced by pH-independent cyclic voltammetry test. Moreover, RuO2/MnO2 sustains its acidic OER activity within 20 h, longer than commercial RuO2. The membrane electrode assembly (MEA) test suggests than only 2.18 V is required to achieve a current density of 5 A/cm2. The theoretical calculation reveals that the eg filling of Ru atom is increased from 2.18 to 2.39 after MnO2 incorporation, reducing the energy for the formation of *OOH moiety.
{"title":"Engineering eg filling of RuO2 enables a robust and stable acidic water oxidation","authors":"Qing Li , Yumei Feng , Yingjie Yu , Yazhou Chen , Yuhua Xie , Fang Luo , Zehui Yang","doi":"10.1016/j.cclet.2024.110612","DOIUrl":"10.1016/j.cclet.2024.110612","url":null,"abstract":"<div><div>Efficient and stable electrocatalyst for oxygen evolution reaction (OER) in acidic environment is vital for polymer electrolyte membrane water electrolysis (PEMWE). In this work, we have devised the formation of heterostructured RuO<sub>2</sub>/MnO<sub>2</sub> with nanoflower structure for acidic OER catalysis. Compared to commercial RuO<sub>2</sub>, the overpotential at 50 mA/cm<sup>2</sup> is decreased by 36 mV, corresponding to a 3.7-fold better mass activity. The boosted acidic OER performance is attributed to the heterostructure inducing more electrons are filled in e<sub>g</sub> orbital of Ru atom triggering a better deprotonation of bridge oxygen atom in Ru-O<sub>bri</sub>-Mn structure evidenced by pH-independent cyclic voltammetry test. Moreover, RuO<sub>2</sub>/MnO<sub>2</sub> sustains its acidic OER activity within 20 h, longer than commercial RuO<sub>2</sub>. The membrane electrode assembly (MEA) test suggests than only 2.18 V is required to achieve a current density of 5 A/cm<sup>2</sup>. The theoretical calculation reveals that the e<sub>g</sub> filling of Ru atom is increased from 2.18 to 2.39 after MnO<sub>2</sub> incorporation, reducing the energy for the formation of *OOH moiety.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 3","pages":"Article 110612"},"PeriodicalIF":9.4,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143318380","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-05DOI: 10.1016/j.cclet.2024.110611
Sanmei Wang , Dengxin Yan , Wenhua Zhang , Liangbing Wang
Manipulating catalyst structures to control product selectivity while maintaining high activity presents a considerable challenge in CO2 hydrogenation. Combining density functional theory calculations and microkinetic analysis, we proposed that graphene-supported isolated Pt atoms (Pt1/graphene) and Pt2 dimers (Pt2/graphene) exhibited distinct selectivity in CO2 hydrogenation. Pt1/graphene facilitated the conversion of CO2 into formic acid, whereas Pt2/graphene favored methanol generation. The variation in product selectivity arose from the synergistic interaction of Pt2 dimers, which facilitated the migration of H atoms between two Pt atoms and promoted the transformation from *COOH intermediates to *C(OH)2 intermediates, altering the reaction pathways compared to isolated Pt atoms. Additionally, an analysis of the catalytic activities of three Pt1/graphene and three Pt2/graphene structures revealed that the turnover frequencies for formic acid generation on Pt1ii/graphene and methanol generation on Pt2i/graphene were as high as 744.48 h-1 and 789.48 h-1, respectively. These values rivaled or even surpassed those previously reported in the literature under identical conditions. This study provides valuable insights into optimizing catalyst structures to achieve desired products in CO2 hydrogenation
{"title":"Graphene-supported isolated platinum atoms and platinum dimers for CO2 hydrogenation: Catalytic activity and selectivity variations","authors":"Sanmei Wang , Dengxin Yan , Wenhua Zhang , Liangbing Wang","doi":"10.1016/j.cclet.2024.110611","DOIUrl":"10.1016/j.cclet.2024.110611","url":null,"abstract":"<div><div>Manipulating catalyst structures to control product selectivity while maintaining high activity presents a considerable challenge in CO<sub>2</sub> hydrogenation. Combining density functional theory calculations and microkinetic analysis, we proposed that graphene-supported isolated Pt atoms (Pt<sub>1</sub>/graphene) and Pt<sub>2</sub> dimers (Pt<sub>2</sub>/graphene) exhibited distinct selectivity in CO<sub>2</sub> hydrogenation. Pt<sub>1</sub>/graphene facilitated the conversion of CO<sub>2</sub> into formic acid, whereas Pt<sub>2</sub>/graphene favored methanol generation. The variation in product selectivity arose from the synergistic interaction of Pt<sub>2</sub> dimers, which facilitated the migration of H atoms between two Pt atoms and promoted the transformation from *COOH intermediates to *C(OH)<sub>2</sub> intermediates, altering the reaction pathways compared to isolated Pt atoms. Additionally, an analysis of the catalytic activities of three Pt<sub>1</sub>/graphene and three Pt<sub>2</sub>/graphene structures revealed that the turnover frequencies for formic acid generation on Pt<sub>1ii</sub>/graphene and methanol generation on Pt<sub>2i</sub>/graphene were as high as 744.48 h<sup>-1</sup> and 789.48 h<sup>-1</sup>, respectively. These values rivaled or even surpassed those previously reported in the literature under identical conditions. This study provides valuable insights into optimizing catalyst structures to achieve desired products in CO<sub>2</sub> hydrogenation</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 4","pages":"Article 110611"},"PeriodicalIF":9.4,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143149443","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-04DOI: 10.1016/j.cclet.2024.110608
Yunxia Liu , Guandong Wu , Lin Li , Yiming Niu , Bingsen Zhang , Botao Qiao , Junhu Wang
Maintaining high metal dispersion of supported metal catalysts to achieve superior reactivity under harsh conditions poses one of the main challenges for their practical applications. Constructing and regulating the strong metal-support interactions (SMSI) by diverse methodologies has emerged as one of the promising approaches to fabricating robust supported metal catalysts. In this study, we report an l-ascorbic acid (AA)-inducing strategy to generate SMSI on a titania-supported gold (Au) catalyst after high-temperature treatment in an inert atmosphere (600 °C, N2). The AA-induced SMSI can efficiently stabilize Au nanoparticles (NPs) and preserve their catalytic performance. The detailed study reveals that the key to realizing this SMSI is the generation of oxygen vacancies within the TiO2 support induced by the adsorbed AA, which drives the formation of the TiOx permeable layer onto the Au NPs. The strategy could be extended to TiO2-supported Au catalysts with different crystal phases and platinum group metals, such as Pt, Pd, and Rh. This work offers a promising novel route to design stable and efficient supported noble metal catalysts by constructing SMSI using simple reducing organic adsorbent.
{"title":"Construction of sintering-resistant gold catalysts via ascorbic-acid inducing strong metal-support interactions","authors":"Yunxia Liu , Guandong Wu , Lin Li , Yiming Niu , Bingsen Zhang , Botao Qiao , Junhu Wang","doi":"10.1016/j.cclet.2024.110608","DOIUrl":"10.1016/j.cclet.2024.110608","url":null,"abstract":"<div><div>Maintaining high metal dispersion of supported metal catalysts to achieve superior reactivity under harsh conditions poses one of the main challenges for their practical applications. Constructing and regulating the strong metal-support interactions (SMSI) by diverse methodologies has emerged as one of the promising approaches to fabricating robust supported metal catalysts. In this study, we report an <span>l</span>-ascorbic acid (AA)-inducing strategy to generate SMSI on a titania-supported gold (Au) catalyst after high-temperature treatment in an inert atmosphere (600 °C, N2). The AA-induced SMSI can efficiently stabilize Au nanoparticles (NPs) and preserve their catalytic performance. The detailed study reveals that the key to realizing this SMSI is the generation of oxygen vacancies within the TiO<sub>2</sub> support induced by the adsorbed AA, which drives the formation of the TiO<sub><em>x</em></sub> permeable layer onto the Au NPs. The strategy could be extended to TiO<sub>2</sub>-supported Au catalysts with different crystal phases and platinum group metals, such as Pt, Pd, and Rh. This work offers a promising novel route to design stable and efficient supported noble metal catalysts by constructing SMSI using simple reducing organic adsorbent.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 4","pages":"Article 110608"},"PeriodicalIF":9.4,"publicationDate":"2024-11-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143149390","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-03DOI: 10.1016/j.cclet.2024.110602
Zhiqiang Wang , Yajie Gao , Tianjun Wang , Wei Chen , Zefeng Ren , Xueming Yang , Chuanyao Zhou
The oxygen evolution reaction (OER) is the bottleneck in the overall photocatalytic splitting of water. The active sites (terminal titanium or bridging oxygen) and active species (molecular or dissociative water) of the initial step of the photocatalyzed OER on the prototypical photocatalyst TiO2, remain debatable. Herein, the photocatalytic chemistry of monolayer water on oxygen-pretreated TiO2(110) (o-TiO2(110)) and reduced TiO2(110) (r-TiO2(110)) surfaces initiated by 400 nm light illumination was investigated by time-dependent two-photon photoemission spectroscopy (TD-2PPE). The photoinduced reduction of the H2O/o-TiO2(110) interface rather than the H2O/r-TiO2(110) interface was detected by TD-2PPE. The difference in 2PPE originated from the presence of the terminal hydroxyl anions (OHt¯) on H2O/o-TiO2(110), as identified by X-ray photoelectron spectroscopy and temperature-programmed desorption. Therefore, the evolution of the electronic structure of H2O/o-TiO2(110) was attributed to the photocatalyzed oxidation of the terminal hydroxyl anions, which most likely formed gaseous •OH radicals, reducing the interface. This work suggested that the oxidation of hydroxyl anions on top of the terminal titanium ions on TiO2, which were excluded previously in solution, need to be considered in the mechanistic studies of the photocatalyzed OER.
{"title":"Photocatalyzed oxidation of water on oxygen pretreated rutile TiO2(110)","authors":"Zhiqiang Wang , Yajie Gao , Tianjun Wang , Wei Chen , Zefeng Ren , Xueming Yang , Chuanyao Zhou","doi":"10.1016/j.cclet.2024.110602","DOIUrl":"10.1016/j.cclet.2024.110602","url":null,"abstract":"<div><div>The oxygen evolution reaction (OER) is the bottleneck in the overall photocatalytic splitting of water. The active sites (terminal titanium or bridging oxygen) and active species (molecular or dissociative water) of the initial step of the photocatalyzed OER on the prototypical photocatalyst TiO<sub>2</sub>, remain debatable. Herein, the photocatalytic chemistry of monolayer water on oxygen-pretreated TiO<sub>2</sub>(110) (<em>o</em>-TiO<sub>2</sub>(110)) and reduced TiO<sub>2</sub>(110) (<em>r</em>-TiO<sub>2</sub>(110)) surfaces initiated by 400 nm light illumination was investigated by time-dependent two-photon photoemission spectroscopy (TD-2PPE). The photoinduced reduction of the H<sub>2</sub>O/<em>o</em>-TiO<sub>2</sub>(110) interface rather than the H<sub>2</sub>O/<em>r</em>-TiO<sub>2</sub>(110) interface was detected by TD-2PPE. The difference in 2PPE originated from the presence of the terminal hydroxyl anions (OH<sub>t</sub>¯) on H<sub>2</sub>O/<em>o</em>-TiO<sub>2</sub>(110), as identified by X-ray photoelectron spectroscopy and temperature-programmed desorption. Therefore, the evolution of the electronic structure of H<sub>2</sub>O/<em>o</em>-TiO<sub>2</sub>(110) was attributed to the photocatalyzed oxidation of the terminal hydroxyl anions, which most likely formed gaseous <sup>•</sup>OH radicals, reducing the interface. This work suggested that the oxidation of hydroxyl anions on top of the terminal titanium ions on TiO<sub>2</sub>, which were excluded previously in solution, need to be considered in the mechanistic studies of the photocatalyzed OER.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 4","pages":"Article 110602"},"PeriodicalIF":9.4,"publicationDate":"2024-11-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143098579","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-01DOI: 10.1016/j.cclet.2024.110604
Xuanyang Jin, Xincheng Guo, Siyang Dong, Shilan Li, Shengdong Jin, Peng Xia, Shengjun Lu, Yufei Zhang, Haosen Fan
Lithium-sulfur batteries (LSBs) are considered as the most promising energy storage technologies owing to their large theoretical energy density (2500 Wh/kg) and specific capacity (1675 mAh/g). However, the heavy shuttle effect of polysulfides and the growth of lithium dendrites greatly hinder their further development and commercial application. In this paper, cobalt-molybdenum bimetallic carbides heterostructure (Co6Mo6C2@Co@NC) was successfully prepared through chemical etching procedure of ZIF-67 precursor with sodium molybdate and the subsequent high temperature annealing process. The obtained dodecahedral Co6Mo6C2@Co@NC with hollow and porous structure provides large specific surface area and plentiful active sites, which speeds up the chemisorption and catalytic conversion of polysulfides, thus mitigating the shuttle effect of polysulfides and the generation of lithium dendrites. When applied as the LSBs separator modifier layer, the cell with modified separator present excellent rate capability and durable cycling stability. In particular, the cell with Co6Mo6C2@Co@NC/PP separator can maintain the high capacity of 738 mAh/g at the current density of 2 C and the specific capacity of 782.6 mAh/g after 300 cycles at 0.5 C, with the coulombic efficiency (CE) near to 100%. Moreover, the Co6Mo6C2@Co@NC/PP battery exhibits the impressive capacity of 431 mAh/g in high sulfur loading (4.096 mg/cm2) at 0.5 C after 200 cycles. This work paves the way for the development of bimetallic carbides heterostructure multifunctional catalysts for durable Li-S battery applications and reveals the synergistic regulation of polysulfides and lithium dendrites through the optimization of the structure and composition.
{"title":"Synergistic regulation of polysulfides shuttle effect and lithium dendrites from cobalt-molybdenum bimetallic carbides (Co-Mo-C) heterostructure for robust Li-S batteries","authors":"Xuanyang Jin, Xincheng Guo, Siyang Dong, Shilan Li, Shengdong Jin, Peng Xia, Shengjun Lu, Yufei Zhang, Haosen Fan","doi":"10.1016/j.cclet.2024.110604","DOIUrl":"https://doi.org/10.1016/j.cclet.2024.110604","url":null,"abstract":"Lithium-sulfur batteries (LSBs) are considered as the most promising energy storage technologies owing to their large theoretical energy density (2500 Wh/kg) and specific capacity (1675 mAh/g). However, the heavy shuttle effect of polysulfides and the growth of lithium dendrites greatly hinder their further development and commercial application. In this paper, cobalt-molybdenum bimetallic carbides heterostructure (Co<sub>6</sub>Mo<sub>6</sub>C<sub>2</sub>@Co@NC) was successfully prepared through chemical etching procedure of ZIF-67 precursor with sodium molybdate and the subsequent high temperature annealing process. The obtained dodecahedral Co<sub>6</sub>Mo<sub>6</sub>C<sub>2</sub>@Co@NC with hollow and porous structure provides large specific surface area and plentiful active sites, which speeds up the chemisorption and catalytic conversion of polysulfides, thus mitigating the shuttle effect of polysulfides and the generation of lithium dendrites. When applied as the LSBs separator modifier layer, the cell with modified separator present excellent rate capability and durable cycling stability. In particular, the cell with Co<sub>6</sub>Mo<sub>6</sub>C<sub>2</sub>@Co@NC/PP separator can maintain the high capacity of 738 mAh/g at the current density of 2 C and the specific capacity of 782.6 mAh/g after 300 cycles at 0.5 C, with the coulombic efficiency (CE) near to 100%. Moreover, the Co<sub>6</sub>Mo<sub>6</sub>C<sub>2</sub>@Co@NC/PP battery exhibits the impressive capacity of 431 mAh/g in high sulfur loading (4.096 mg/cm<sup>2</sup>) at 0.5 C after 200 cycles. This work paves the way for the development of bimetallic carbides heterostructure multifunctional catalysts for durable Li-S battery applications and reveals the synergistic regulation of polysulfides and lithium dendrites through the optimization of the structure and composition.","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"79 1","pages":""},"PeriodicalIF":9.1,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142562363","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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