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Novel NIR-II 3,5-Julolidinyl aza-BODIPY for Photothermal Therapy of Gliomas Stem Cells by Brain Stereotactic Injection 通过脑立体定向注射对胶质瘤干细胞进行光热治疗的新型 NIR-II 3,5-Julolidinyl aza-BODIPY
IF 11.4 1区 化学
ACS Materials Letters Pub Date : 2024-09-20 DOI: 10.1021/acsmaterialslett.4c01447
Lulu Cao, Zhiqiang Cui, Dongxiang Zhang, Yikun Li, Xiaoyan Gao, Rong Shang, Xin-Dong Jiang, Jianjun Du, Xiaohong Sun
{"title":"Novel NIR-II 3,5-Julolidinyl aza-BODIPY for Photothermal Therapy of Gliomas Stem Cells by Brain Stereotactic Injection","authors":"Lulu Cao, Zhiqiang Cui, Dongxiang Zhang, Yikun Li, Xiaoyan Gao, Rong Shang, Xin-Dong Jiang, Jianjun Du, Xiaohong Sun","doi":"10.1021/acsmaterialslett.4c01447","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c01447","url":null,"abstract":"Functional dyes with absorption in the second near-infrared window (NIR-II) show great promise in photothermal therapy. Herein, the novel NIR-II 3,5-julolidinyl aza-BODIPY (<b>JLD</b>) was prepared and confirmed by X-ray crystallographic analysis for the first time. The molecular packing structure facilitates the <i>J</i>-aggregation packing mode. Self-assembled <b>JLD</b>-nanoparticles (<b>JLD</b>-NPs) emit fluorescence (λ<sub>em</sub> = 962 nm, Φ<sub>f</sub> = 0.1%), and a peak belt covered a NIR-II range of 900–1300 nm. The photothermal conversion efficiency was high and was calculated to be 79%. <b>JLD</b>-NPs with NIR-II 915 nm laser irradiation had the good tumor-inhibition capability with promoting the apoptosis and inhibiting the stemness of glioblastoma cells by brain stereotactic injection and affect the occurrence of malignant events, such as migration and invasion.","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":null,"pages":null},"PeriodicalIF":11.4,"publicationDate":"2024-09-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142251697","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}
引用次数: 0
Tailoring Surface Electronic Structure of Spinel Co3O4 Oxide via Fe and Cu Substitution for Enhanced Oxygen Evolution Reaction 通过铁和铜置换调整尖晶石 Co3O4 氧化物的表面电子结构以增强氧进化反应
IF 11.4 1区 化学
ACS Materials Letters Pub Date : 2024-09-20 DOI: 10.1021/acsmaterialslett.4c00857
Mahmoud G. Ahmed, Ying Fan Tay, Mengyuan Zhang, Sing Yang Chiam, Lydia H. Wong
{"title":"Tailoring Surface Electronic Structure of Spinel Co3O4 Oxide via Fe and Cu Substitution for Enhanced Oxygen Evolution Reaction","authors":"Mahmoud G. Ahmed, Ying Fan Tay, Mengyuan Zhang, Sing Yang Chiam, Lydia H. Wong","doi":"10.1021/acsmaterialslett.4c00857","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c00857","url":null,"abstract":"Multimetal spinel oxides are promising candidates for the oxygen evolution reaction (OER) due to their ability to offer more accessible active sites and oxygen vacancies (O<sub>vac</sub>). However, the utilization of redox-active species in spinel oxides is limited. Herein, we unveil an efficient multimetal spinel oxide using high-throughput methods. The oxide contains Fe and Cu substituted into Co sites following a stoichiometry of Fe<sub>0.6</sub>Cu<sub>0.6</sub>Co<sub>1.8</sub>O<sub>4</sub>. The dual cation substitution of Fe and Cu manipulates the electronic states and generates O<sub>vac</sub>, thereby generating more accessible active species. This significantly improves the OH<sup>–</sup> adsorption capacity on spinel oxide triggering a more favorable OER reaction with a low overpotential of 265 mV at 10 mA cm<sup>–2</sup> and high durability in an alkaline medium. Our work not only presents the utilization of a high-throughput approach to explore efficient catalysts with optimal composition but also provides useful insights into the modulation of electronic states for enhanced catalytic performance.","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":null,"pages":null},"PeriodicalIF":11.4,"publicationDate":"2024-09-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142251695","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}
引用次数: 0
New Concept for HLCT Emitter: Acceptor Molecule in Exciplex System for Highly Efficient and Extremely Low-Efficiency Roll-Off Solution-Processed OLED HLCT 发射器的新概念:用于高效和极低效率滚降溶液加工型有机发光二极管的复合系统中的受体分子
IF 11.4 1区 化学
ACS Materials Letters Pub Date : 2024-09-19 DOI: 10.1021/acsmaterialslett.4c01643
Yixiao Yin, Yinyan Wu, Binghong He, Zekun Xia, Weiguo Zhu, Jun Yeob Lee, Yafei Wang
{"title":"New Concept for HLCT Emitter: Acceptor Molecule in Exciplex System for Highly Efficient and Extremely Low-Efficiency Roll-Off Solution-Processed OLED","authors":"Yixiao Yin, Yinyan Wu, Binghong He, Zekun Xia, Weiguo Zhu, Jun Yeob Lee, Yafei Wang","doi":"10.1021/acsmaterialslett.4c01643","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c01643","url":null,"abstract":"The use of hybridized local and charge-transfer (HLCT) emitters as acceptor or donor molecules in exciplex systems is still a novel concept even though HLCT molecules can harvest both singlet and triplet excitons. Herein, two HLCT emitters, 2-<sup><i>t</i></sup>Bu<i>spo</i>Cz-2pTrz and 2-<sup><i>t</i></sup>Bu<i>spo</i>Cz-Me3pTrz, are prepared as acceptors of exciplexes with thermally activated delayed fluorescence (TADF) properties. The exciplex TADF systems constructed by mixing HLCT and TAPC molecules have a minute energy gap between singlet and triplet excited states and unity emission efficiency. Using the exciplex as an emitter, solution-processed devices achieve maximum external quantum efficiency (<i>EQE</i><sub>max</sub>) of 16.6%. Impressively, solution-processed devices with the fabricated exciplexes as hosts exhibit extremely low turn-on voltages and a promising <i>EQE</i><sub>max</sub> of &gt;20%, which is concomitant with an extremely low-efficiency roll-off of 0.5% at 1,000 cd m<sup>–2</sup>. This study explores the potential of HLCT emitters as acceptors of exciplexes and guides the design of efficient exciplex systems.","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":null,"pages":null},"PeriodicalIF":11.4,"publicationDate":"2024-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142251698","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}
引用次数: 0
New Concept for HLCT Emitter: Acceptor Molecule in Exciplex System for Highly Efficient and Extremely Low-Efficiency Roll-Off Solution-Processed OLED HLCT 发射器的新概念:用于高效和极低效率滚降溶液加工型有机发光二极管的复合系统中的受体分子
IF 9.6 1区 化学
ACS Materials Letters Pub Date : 2024-09-19 DOI: 10.1021/acsmaterialslett.4c0164310.1021/acsmaterialslett.4c01643
Yixiao Yin, Yinyan Wu, Binghong He, Zekun Xia, Weiguo Zhu, Jun Yeob Lee* and Yafei Wang*, 
{"title":"New Concept for HLCT Emitter: Acceptor Molecule in Exciplex System for Highly Efficient and Extremely Low-Efficiency Roll-Off Solution-Processed OLED","authors":"Yixiao Yin,&nbsp;Yinyan Wu,&nbsp;Binghong He,&nbsp;Zekun Xia,&nbsp;Weiguo Zhu,&nbsp;Jun Yeob Lee* and Yafei Wang*,&nbsp;","doi":"10.1021/acsmaterialslett.4c0164310.1021/acsmaterialslett.4c01643","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c01643https://doi.org/10.1021/acsmaterialslett.4c01643","url":null,"abstract":"<p >The use of hybridized local and charge-transfer (HLCT) emitters as acceptor or donor molecules in exciplex systems is still a novel concept even though HLCT molecules can harvest both singlet and triplet excitons. Herein, two HLCT emitters, 2-<sup><i>t</i></sup>Bu<i>spo</i>Cz-2pTrz and 2-<sup><i>t</i></sup>Bu<i>spo</i>Cz-Me3pTrz, are prepared as acceptors of exciplexes with thermally activated delayed fluorescence (TADF) properties. The exciplex TADF systems constructed by mixing HLCT and TAPC molecules have a minute energy gap between singlet and triplet excited states and unity emission efficiency. Using the exciplex as an emitter, solution-processed devices achieve maximum external quantum efficiency (<i>EQE</i><sub>max</sub>) of 16.6%. Impressively, solution-processed devices with the fabricated exciplexes as hosts exhibit extremely low turn-on voltages and a promising <i>EQE</i><sub>max</sub> of &gt;20%, which is concomitant with an extremely low-efficiency roll-off of 0.5% at 1,000 cd m<sup>–2</sup>. This study explores the potential of HLCT emitters as acceptors of exciplexes and guides the design of efficient exciplex systems.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":null,"pages":null},"PeriodicalIF":9.6,"publicationDate":"2024-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142403006","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}
引用次数: 0
Construction of Sulfur Doped Nickel and Copper Interfaces for Hydrogen Evolution Reaction 构建用于氢气进化反应的掺硫镍铜界面
IF 11.4 1区 化学
ACS Materials Letters Pub Date : 2024-09-18 DOI: 10.1021/acsmaterialslett.4c01339
Jiajie Yu, Shiwen Zhang, Yuyang Liu, Yurun Tong, Yijie Zhong, Bin He, Enlai Hu, Jing Zhang, Zhongwei Chen
{"title":"Construction of Sulfur Doped Nickel and Copper Interfaces for Hydrogen Evolution Reaction","authors":"Jiajie Yu, Shiwen Zhang, Yuyang Liu, Yurun Tong, Yijie Zhong, Bin He, Enlai Hu, Jing Zhang, Zhongwei Chen","doi":"10.1021/acsmaterialslett.4c01339","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c01339","url":null,"abstract":"Developing efficient and economical electrocatalysts for the hydrogen evolution reaction (HER) is important for high-purity hydrogen generation. Transition metals-based compounds have been considered as promising substitutes for the Pt-based electrocatalysts toward HER. Nevertheless, pure metals display inert HER activity because of their unfavorable adsorption behavior for intermediates. Herein, thiourea engaged electrodeposition was conducted to fabricate sulfur-doped nickel and copper (S–Ni/Cu) nanowires that contain numerous interfaces. Interface and sulfur doping redistributed the electronic states of the electrocatalyst structure, which accelerated the adsorption of hydrogen atoms at active sites and promoted the water dissociation process. Consequently, the HER overpotential of S–Ni/Cu is only 67 mV at 10 mA cm<sup>–2</sup>, with excellent durability.","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":null,"pages":null},"PeriodicalIF":11.4,"publicationDate":"2024-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142251700","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}
引用次数: 0
Realization of Evaporated Electrode-Based Intrinsically Stretchable Ternary Organic Solar Cells through Encapsulation Strategy 通过封装策略实现基于蒸发电极的本征可拉伸三元有机太阳能电池
IF 11.4 1区 化学
ACS Materials Letters Pub Date : 2024-09-18 DOI: 10.1021/acsmaterialslett.4c01548
Zhenye Wang, Di Zhang, Lvpeng Yang, Meichen Xu, Junfeng Liu, Zhi Wang, Yerun Gao, Li-Yuan Zhang, Lianbin Niu, Ming Shao
{"title":"Realization of Evaporated Electrode-Based Intrinsically Stretchable Ternary Organic Solar Cells through Encapsulation Strategy","authors":"Zhenye Wang, Di Zhang, Lvpeng Yang, Meichen Xu, Junfeng Liu, Zhi Wang, Yerun Gao, Li-Yuan Zhang, Lianbin Niu, Ming Shao","doi":"10.1021/acsmaterialslett.4c01548","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c01548","url":null,"abstract":"The mechanical properties of organic solar cells are of great importance to ensure their application in wearable or stretchable electronics. Here, we introduce polymer acceptor (N2200) into the active layer blend, and realize intrinsically stretchable organic solar cells (<i>is</i>-OSCs) with evaporated electrode via encapsulation strategy. The incorporation of N2200 simultaneously enhances the mechanical stretchability and PCE of <i>is</i>-OSCs, attributed to the enhanced polymer chain entanglement, and N2200 can act as tie molecules to provide electric connection among small molecule domains. More importantly, encapsulating the evaporated electrode-based <i>is</i>-OSCs leads to significant improvement in its mechanical stretchability, with 80% PCE retention under a large strain of 20%, compared to &lt;2.5% strain for the unencapsulated ones. Additionally, encapsulated <i>is</i>-OSCs retained 67% PCE after 1000 test cycles at a stretch strain of 15%, whereas unencapsulated devices can only retain 33% PCE after 200 test cycles under a small strain of 5%.","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":null,"pages":null},"PeriodicalIF":11.4,"publicationDate":"2024-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142251732","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}
引用次数: 0
Realization of Evaporated Electrode-Based Intrinsically Stretchable Ternary Organic Solar Cells through Encapsulation Strategy 通过封装策略实现基于蒸发电极的本征可拉伸三元有机太阳能电池
IF 9.6 1区 化学
ACS Materials Letters Pub Date : 2024-09-18 DOI: 10.1021/acsmaterialslett.4c0154810.1021/acsmaterialslett.4c01548
Zhenye Wang, Di Zhang, Lvpeng Yang, Meichen Xu, Junfeng Liu, Zhi Wang, Yerun Gao, Li-Yuan Zhang, Lianbin Niu and Ming Shao*, 
{"title":"Realization of Evaporated Electrode-Based Intrinsically Stretchable Ternary Organic Solar Cells through Encapsulation Strategy","authors":"Zhenye Wang,&nbsp;Di Zhang,&nbsp;Lvpeng Yang,&nbsp;Meichen Xu,&nbsp;Junfeng Liu,&nbsp;Zhi Wang,&nbsp;Yerun Gao,&nbsp;Li-Yuan Zhang,&nbsp;Lianbin Niu and Ming Shao*,&nbsp;","doi":"10.1021/acsmaterialslett.4c0154810.1021/acsmaterialslett.4c01548","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c01548https://doi.org/10.1021/acsmaterialslett.4c01548","url":null,"abstract":"<p >The mechanical properties of organic solar cells are of great importance to ensure their application in wearable or stretchable electronics. Here, we introduce polymer acceptor (N2200) into the active layer blend, and realize intrinsically stretchable organic solar cells (<i>is</i>-OSCs) with evaporated electrode via encapsulation strategy. The incorporation of N2200 simultaneously enhances the mechanical stretchability and PCE of <i>is</i>-OSCs, attributed to the enhanced polymer chain entanglement, and N2200 can act as tie molecules to provide electric connection among small molecule domains. More importantly, encapsulating the evaporated electrode-based <i>is</i>-OSCs leads to significant improvement in its mechanical stretchability, with 80% PCE retention under a large strain of 20%, compared to &lt;2.5% strain for the unencapsulated ones. Additionally, encapsulated <i>is</i>-OSCs retained 67% PCE after 1000 test cycles at a stretch strain of 15%, whereas unencapsulated devices can only retain 33% PCE after 200 test cycles under a small strain of 5%.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":null,"pages":null},"PeriodicalIF":9.6,"publicationDate":"2024-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142407668","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}
引用次数: 0
Construction of Sulfur Doped Nickel and Copper Interfaces for Hydrogen Evolution Reaction 构建用于氢气进化反应的掺硫镍铜界面
IF 9.6 1区 化学
ACS Materials Letters Pub Date : 2024-09-18 DOI: 10.1021/acsmaterialslett.4c0133910.1021/acsmaterialslett.4c01339
Jiajie Yu, Shiwen Zhang, Yuyang Liu, Yurun Tong, Yijie Zhong, Bin He, Enlai Hu*, Jing Zhang* and Zhongwei Chen*, 
{"title":"Construction of Sulfur Doped Nickel and Copper Interfaces for Hydrogen Evolution Reaction","authors":"Jiajie Yu,&nbsp;Shiwen Zhang,&nbsp;Yuyang Liu,&nbsp;Yurun Tong,&nbsp;Yijie Zhong,&nbsp;Bin He,&nbsp;Enlai Hu*,&nbsp;Jing Zhang* and Zhongwei Chen*,&nbsp;","doi":"10.1021/acsmaterialslett.4c0133910.1021/acsmaterialslett.4c01339","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c01339https://doi.org/10.1021/acsmaterialslett.4c01339","url":null,"abstract":"<p >Developing efficient and economical electrocatalysts for the hydrogen evolution reaction (HER) is important for high-purity hydrogen generation. Transition metals-based compounds have been considered as promising substitutes for the Pt-based electrocatalysts toward HER. Nevertheless, pure metals display inert HER activity because of their unfavorable adsorption behavior for intermediates. Herein, thiourea engaged electrodeposition was conducted to fabricate sulfur-doped nickel and copper (S–Ni/Cu) nanowires that contain numerous interfaces. Interface and sulfur doping redistributed the electronic states of the electrocatalyst structure, which accelerated the adsorption of hydrogen atoms at active sites and promoted the water dissociation process. Consequently, the HER overpotential of S–Ni/Cu is only 67 mV at 10 mA cm<sup>–2</sup>, with excellent durability.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":null,"pages":null},"PeriodicalIF":9.6,"publicationDate":"2024-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142402822","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}
引用次数: 0
Fabrication of Cu–CeO2 Catalyst with Abundant Interfacial Cu+–O–Ce3+–OV (Oxygen Vacancy) Sites for Boosting CO2 Electroreduction to Methane 制备具有丰富表面 Cu+-O-Ce3+-OV(氧空位)位点的 Cu-CeO2 催化剂,促进 CO2 电还原为甲烷
IF 9.6 1区 化学
ACS Materials Letters Pub Date : 2024-09-18 DOI: 10.1021/acsmaterialslett.4c0168310.1021/acsmaterialslett.4c01683
Shao-Chen Wang, Xiang Ji, Rui Hou, Longlong Qi, Peng Jing, Xuan Xu, Baocang Liu* and Jun Zhang*, 
{"title":"Fabrication of Cu–CeO2 Catalyst with Abundant Interfacial Cu+–O–Ce3+–OV (Oxygen Vacancy) Sites for Boosting CO2 Electroreduction to Methane","authors":"Shao-Chen Wang,&nbsp;Xiang Ji,&nbsp;Rui Hou,&nbsp;Longlong Qi,&nbsp;Peng Jing,&nbsp;Xuan Xu,&nbsp;Baocang Liu* and Jun Zhang*,&nbsp;","doi":"10.1021/acsmaterialslett.4c0168310.1021/acsmaterialslett.4c01683","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c01683https://doi.org/10.1021/acsmaterialslett.4c01683","url":null,"abstract":"<p >Accelerating the conversion of *CO to *CHO and promoting the adsorption and hydrogenation of *CHO are the keys to achieving a highly selective electrocatalytic CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR) to CH<sub>4</sub> over Cu-based catalysts. Herein, a novel electrocatalyst comprising highly dispersed Cu nanoclusters (Cu<sub>NCs</sub>) supported on oxygen vacancy (O<sub>V</sub>)-rich CeO<sub>2</sub> on carbon paper (Cu<sub>NCs</sub>–CeO<sub>2</sub>/CP) with plentiful interfacial Cu<sup>+</sup>–O–Ce<sup>3+</sup>–O<sub>V</sub> sites is constructed via a facile electrodeposition method. Various <i>in situ</i>/<i>ex situ</i> characterizations and theoretical calculations unveil that the Cu<sup>+</sup>–O–Ce<sup>3+</sup>–O<sub>V</sub> sites can effectively regulate the pathway of the CO<sub>2</sub>RR, accelerate the *CO → *CHO process, stabilize the *CHO and *OCH<sub>3</sub> intermediates, and promote their hydrogenation to produce CH<sub>4</sub>. Furthermore, the critical role of Ce<sup>3+</sup> and the O<sub>V</sub> species in forming Cu<sup>+</sup>–O–Ce<sup>3+</sup>–O<sub>V</sub> to maintain the electrocatalytic CO<sub>2</sub>RR activity is revealed. The optimized Cu<sub>NCs</sub>–CeO<sub>2</sub>/CP electrocatalyst exhibits a CH<sub>4</sub> Faradaic efficiency of 68.3% at 500 mA cm<sup>–2</sup>, with a high partial current density of 340 mA cm<sup>–2</sup>.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":null,"pages":null},"PeriodicalIF":9.6,"publicationDate":"2024-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142407758","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}
引用次数: 0
Fabrication of Cu–CeO2 Catalyst with Abundant Interfacial Cu+–O–Ce3+–OV (Oxygen Vacancy) Sites for Boosting CO2 Electroreduction to Methane 制备具有丰富表面 Cu+-O-Ce3+-OV(氧空位)位点的 Cu-CeO2 催化剂,促进 CO2 电还原为甲烷
IF 11.4 1区 化学
ACS Materials Letters Pub Date : 2024-09-18 DOI: 10.1021/acsmaterialslett.4c01683
Shao-Chen Wang, Xiang Ji, Rui Hou, Longlong Qi, Peng Jing, Xuan Xu, Baocang Liu, Jun Zhang
{"title":"Fabrication of Cu–CeO2 Catalyst with Abundant Interfacial Cu+–O–Ce3+–OV (Oxygen Vacancy) Sites for Boosting CO2 Electroreduction to Methane","authors":"Shao-Chen Wang, Xiang Ji, Rui Hou, Longlong Qi, Peng Jing, Xuan Xu, Baocang Liu, Jun Zhang","doi":"10.1021/acsmaterialslett.4c01683","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c01683","url":null,"abstract":"Accelerating the conversion of *CO to *CHO and promoting the adsorption and hydrogenation of *CHO are the keys to achieving a highly selective electrocatalytic CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR) to CH<sub>4</sub> over Cu-based catalysts. Herein, a novel electrocatalyst comprising highly dispersed Cu nanoclusters (Cu<sub>NCs</sub>) supported on oxygen vacancy (O<sub>V</sub>)-rich CeO<sub>2</sub> on carbon paper (Cu<sub>NCs</sub>–CeO<sub>2</sub>/CP) with plentiful interfacial Cu<sup>+</sup>–O–Ce<sup>3+</sup>–O<sub>V</sub> sites is constructed via a facile electrodeposition method. Various <i>in situ</i>/<i>ex situ</i> characterizations and theoretical calculations unveil that the Cu<sup>+</sup>–O–Ce<sup>3+</sup>–O<sub>V</sub> sites can effectively regulate the pathway of the CO<sub>2</sub>RR, accelerate the *CO → *CHO process, stabilize the *CHO and *OCH<sub>3</sub> intermediates, and promote their hydrogenation to produce CH<sub>4</sub>. Furthermore, the critical role of Ce<sup>3+</sup> and the O<sub>V</sub> species in forming Cu<sup>+</sup>–O–Ce<sup>3+</sup>–O<sub>V</sub> to maintain the electrocatalytic CO<sub>2</sub>RR activity is revealed. The optimized Cu<sub>NCs</sub>–CeO<sub>2</sub>/CP electrocatalyst exhibits a CH<sub>4</sub> Faradaic efficiency of 68.3% at 500 mA cm<sup>–2</sup>, with a high partial current density of 340 mA cm<sup>–2</sup>.","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":null,"pages":null},"PeriodicalIF":11.4,"publicationDate":"2024-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142251733","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}
引用次数: 0
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