Pub Date : 2025-10-01DOI: 10.1016/j.cclet.2025.111928
Xinwei Hu , Yong Zeng , Jiongdong Ma , Han Diao , Fei-Xiao Chen , Mu Chen , Shou-Kun Zhang , Chengzhi Jin , Shao-Fei Ni , Zhixiong Ruan
Benzo[b]furans are significant scaffolds in drug molecules and are prevalent structural components in natural products. Chemically encoded non-natural peptidomimetics have a substantial impact on pharmaceuticals by offering enhanced stability, improved cell permeability, and resistance to enzymatic degradation. Consequently, a strategy for the sustainable assembly of benzo[b]furan/benzopyran-functionalized peptides through the electrochemical late-stage modification of alkyne-modified tyrosine oligopeptides is proposed. This approach facilitates the multifunctional integration of non-native tyrosine-derived substrates, as well as their subsequent functionalization. Notably, the resulting peptides exhibit favorable properties regarding biocompatibility and cellular uptake.
{"title":"Electrochemical selenylation of tyrosine oligopeptides to benzo[b]furan-functionalized peptides","authors":"Xinwei Hu , Yong Zeng , Jiongdong Ma , Han Diao , Fei-Xiao Chen , Mu Chen , Shou-Kun Zhang , Chengzhi Jin , Shao-Fei Ni , Zhixiong Ruan","doi":"10.1016/j.cclet.2025.111928","DOIUrl":"10.1016/j.cclet.2025.111928","url":null,"abstract":"<div><div>Benzo[<em>b</em>]furans are significant scaffolds in drug molecules and are prevalent structural components in natural products. Chemically encoded non-natural peptidomimetics have a substantial impact on pharmaceuticals by offering enhanced stability, improved cell permeability, and resistance to enzymatic degradation. Consequently, a strategy for the sustainable assembly of benzo[<em>b</em>]furan/benzopyran-functionalized peptides through the electrochemical late-stage modification of alkyne-modified tyrosine oligopeptides is proposed. This approach facilitates the multifunctional integration of non-native tyrosine-derived substrates, as well as their subsequent functionalization. Notably, the resulting peptides exhibit favorable properties regarding biocompatibility and cellular uptake.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"37 3","pages":"Article 111928"},"PeriodicalIF":8.9,"publicationDate":"2025-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145735511","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 : 2025-10-01DOI: 10.1016/j.cclet.2025.111933
Hongchao Wang , Wei Hao , Haowei Wu , Qianyu Ding , Yu Wei , Hu Zhao , Shuzhou Li , Hanying Li , Jia Zhu
Charge-transfer complexes (CTCs) have emerged as promising n-type organic thermoelectric (TE) materials due to their inherent high electrical conductivity and tunable transport polarities. In this study, we performed a comprehensive first-principles investigation on the TE properties of nine CTCs comprised of 2,7-dialkyl[1]benzothieno[3,2-b][1]benzothiophenes (CnBTBT, n = 4, 8, 12) as donors and fluorinated derivatives of tetracyanoquinodimethane (FmTCNQ, m = 0, 2, 4) as acceptors, aiming to identify high-performance n-type organic TE materials and elucidate the underlying structure–property relationships. Our calculation results, based on the Boltzmann transport equation and deformation potential theory, reveal that the length of the alkyl side chains and the number of fluorine substitutions significantly impact their electronic structures and TE properties. Notably, the CnBTBT–FmTCNQ CTCs with shorter alkyl chains and more fluorine substitution demonstrate superior n-type characteristics, particularly C4BTBT–F4TCNQ, which achieves an excellent power factor of 671 μW cm-1 K-2 at an optimal charge carrier concentration. Our findings not only clarify the critical role of molecular engineering in CTC-based TE materials but also provide valuable guidance for developing high-efficiency organic TE materials with versatile practical applications.
电荷转移配合物（ctc）由于其固有的高导电性和可调的输运极性而成为有前途的n型有机热电（TE）材料。在本研究中，我们对以2,7-二烷基[1]苯并噻吩[3,2-b][1]苯并噻吩（CnBTBT, n = 4,8,12）为给体，以四氰喹二甲烷的氟化衍生物（FmTCNQ, m = 0,2,4）为受体组成的九种ctc的TE性质进行了全面的第一性原理研究，旨在鉴定高性能n型有机TE材料并阐明其潜在的结构-性质关系。我们基于玻尔兹曼输运方程和变形势理论的计算结果表明，烷基侧链的长度和氟取代的数量显著影响它们的电子结构和TE性能。值得注意的是，具有较短烷基链和较多氟取代的CnBTBT-FmTCNQ ctc具有较好的n型特性，特别是C4BTBT-F4TCNQ在最佳载流子浓度下的功率因数为671 μW cm-1 K-2。我们的研究结果不仅阐明了分子工程在ctc基TE材料中的关键作用，而且为开发具有多种实际应用的高效有机TE材料提供了有价值的指导。
{"title":"Rational design of n-type organic thermoelectric materials: Insights from CnBTBT–FmTCNQ charge-transfer complexes","authors":"Hongchao Wang , Wei Hao , Haowei Wu , Qianyu Ding , Yu Wei , Hu Zhao , Shuzhou Li , Hanying Li , Jia Zhu","doi":"10.1016/j.cclet.2025.111933","DOIUrl":"10.1016/j.cclet.2025.111933","url":null,"abstract":"<div><div>Charge-transfer complexes (CTCs) have emerged as promising n-type organic thermoelectric (TE) materials due to their inherent high electrical conductivity and tunable transport polarities. In this study, we performed a comprehensive first-principles investigation on the TE properties of nine CTCs comprised of 2,7-dialkyl[1]benzothieno[3,2-<em>b</em>][1]benzothiophenes (C<em><sub>n</sub></em>BTBT, <em>n</em> = 4, 8, 12) as donors and fluorinated derivatives of tetracyanoquinodimethane (F<em><sub>m</sub></em>TCNQ, <em>m</em> = 0, 2, 4) as acceptors, aiming to identify high-performance n-type organic TE materials and elucidate the underlying structure–property relationships. Our calculation results, based on the Boltzmann transport equation and deformation potential theory, reveal that the length of the alkyl side chains and the number of fluorine substitutions significantly impact their electronic structures and TE properties. Notably, the C<em><sub>n</sub></em>BTBT–F<em><sub>m</sub></em>TCNQ CTCs with shorter alkyl chains and more fluorine substitution demonstrate superior n-type characteristics, particularly C<sub>4</sub>BTBT–F<sub>4</sub>TCNQ, which achieves an excellent power factor of 671 μW cm<sup>-1</sup> K<sup>-2</sup> at an optimal charge carrier concentration. Our findings not only clarify the critical role of molecular engineering in CTC-based TE materials but also provide valuable guidance for developing high-efficiency organic TE materials with versatile practical applications.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"37 2","pages":"Article 111933"},"PeriodicalIF":8.9,"publicationDate":"2025-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145622062","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}
Catalysts are key for olefin polymerization reactions and are also ubiquitous in catalysis science. Multi-nuclear metal catalysts have witnessed enhanced performances in catalytic reactions relative to mono-nuclear catalysts, but which substantially involve multi-step, tedious, and difficult synthesis. Herein, this study reports an intriguing approach to construct multi-nuclear catalysts for the milestone α-diimine nickel catalysts using an oligomeric strategy. A polymerizable norbornene unit is incorporated into the α-diimine ligand backbone, leading to the formation of the monomeric nickel catalyst Ni1 and its corresponding oligomeric nickel catalysts (Ni3 and Ni5) with varying degrees of polymerization (DP = 3 and 5). Notably, the oligomeric catalyst Ni5 was facilely scaled up (50 g-level), showed enhanced thermal stability, exhibited 4.6 times higher activity, and yielded polyethylene elastomer with a 379 % increased molecular weight in ethylene polymerization, compared to the monomeric catalyst Ni1. Catalytic performance enhancements of oligomeric catalysts were found to be DP-dependent. The kilogram-scale polyethylene, produced using Ni5 in a 20 L reactor, presented a highly branched all-hydrocarbon structure, which demonstrated typical elastic properties (tensile strength: 4 MPa, elastic recovery: SR = 72 %) along with great processability (MFI = 3.0 g/10 min), insulating characteristics (volume resistivity = 2 × 1016 Ω/m), and hydrophobicity (water vapor permeability: 0.03 g/m2/day), suggesting potentially practical applications.
{"title":"Oligomeric α-diimine nickel catalysts for enhanced ethylene polymerization","authors":"Jingfeng Yue , Zhenxin Tang , Yuxing Zhang , Zhongbao Jian","doi":"10.1016/j.cclet.2025.111930","DOIUrl":"10.1016/j.cclet.2025.111930","url":null,"abstract":"<div><div>Catalysts are key for olefin polymerization reactions and are also ubiquitous in catalysis science. Multi-nuclear metal catalysts have witnessed enhanced performances in catalytic reactions relative to mono-nuclear catalysts, but which substantially involve multi-step, tedious, and difficult synthesis. Herein, this study reports an intriguing approach to construct multi-nuclear catalysts for the milestone α-diimine nickel catalysts using an oligomeric strategy. A polymerizable norbornene unit is incorporated into the α-diimine ligand backbone, leading to the formation of the monomeric nickel catalyst Ni<sub>1</sub> and its corresponding oligomeric nickel catalysts (Ni<sub>3</sub> and Ni<sub>5</sub>) with varying degrees of polymerization (DP = 3 and 5). Notably, the oligomeric catalyst Ni<sub>5</sub> was facilely scaled up (50 g-level), showed enhanced thermal stability, exhibited 4.6 times higher activity, and yielded polyethylene elastomer with a 379 % increased molecular weight in ethylene polymerization, compared to the monomeric catalyst Ni<sub>1</sub>. Catalytic performance enhancements of oligomeric catalysts were found to be DP-dependent. The kilogram-scale polyethylene, produced using Ni<sub>5</sub> in a 20 L reactor, presented a highly branched all-hydrocarbon structure, which demonstrated typical elastic properties (tensile strength: 4 MPa, elastic recovery: SR = 72 %) along with great processability (MFI = 3.0 g/10 min), insulating characteristics (volume resistivity = 2 × 10<sup>16</sup> Ω/m), and hydrophobicity (water vapor permeability: 0.03 g/m<sup>2</sup>/day), suggesting potentially practical applications.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"37 1","pages":"Article 111930"},"PeriodicalIF":8.9,"publicationDate":"2025-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145339842","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 : 2025-09-30DOI: 10.1016/j.cclet.2025.111926
Min Zhang , Weimin Wang , Jun Li , Xun Zhu , Qian Fu
Developing advanced electrocatalysts to convert CO2 into liquid fuels such as C2H5OH is critical for utilizing intermittent renewable energy. The formation of C2H5OH, however, is generally less favored compared with the other hydrocarbon products from Cu-based electrocatalysts. In this work, an alkanethiol-modified Cu₂O nanowire array (OTT-Cu₂O) was constructed with asymmetric Cu sites consisting of paired Cu–O and Cu–S motifs to overcome previous limitations of C2H5OH electrosynthesis via CO2RR pathway. This catalyst achieves a high Faradaic efficiency of 45 % for CO2-to-C2H5OH conversion at 300 mA/cm2, representing a more than two-fold enhancement over the Cu2O electrode. Mechanistic investigations reveal that the Cu–S site exhibits distinct C-binding capability that stabilizes key intermediates (*OCH2 and *CO), in contrast to the O-affinitive Cu–O site. The asymmetric S–Cu–O configuration promotes thermodynamically favorable asymmetric C–C coupling between *CO and *OCH2, forming the critical CO–OCH₂ intermediate and facilitating C2H5OH production, as opposed to symmetric O–Cu–O sites that mainly generate HCOOH. This work offers an effective strategy for designing multi-active-site catalysts toward highly selective CO₂ reduction to C2H5OH and provides fundamental insight into the reaction mechanism.
{"title":"Efficient large-current conversion of CO2 to C2H5OH via a *CO-*OCH2 coupling pathway on alkanethiol-modified Cu2O array electrode","authors":"Min Zhang , Weimin Wang , Jun Li , Xun Zhu , Qian Fu","doi":"10.1016/j.cclet.2025.111926","DOIUrl":"10.1016/j.cclet.2025.111926","url":null,"abstract":"<div><div>Developing advanced electrocatalysts to convert CO<sub>2</sub> into liquid fuels such as C<sub>2</sub>H<sub>5</sub>OH is critical for utilizing intermittent renewable energy. The formation of C<sub>2</sub>H<sub>5</sub>OH, however, is generally less favored compared with the other hydrocarbon products from Cu-based electrocatalysts. In this work, an alkanethiol-modified Cu₂O nanowire array (OTT-Cu₂O) was constructed with asymmetric Cu sites consisting of paired Cu–O and Cu–S motifs to overcome previous limitations of C<sub>2</sub>H<sub>5</sub>OH electrosynthesis <em>via</em> CO<sub>2</sub>RR pathway. This catalyst achieves a high Faradaic efficiency of 45 % for CO<sub>2</sub>-to-C<sub>2</sub>H<sub>5</sub>OH conversion at 300 mA/cm<sup>2</sup>, representing a more than two-fold enhancement over the Cu<sub>2</sub>O electrode. Mechanistic investigations reveal that the Cu–S site exhibits distinct C-binding capability that stabilizes key intermediates (*OCH<sub>2</sub> and *CO), in contrast to the O-affinitive Cu–O site. The asymmetric S–Cu–O configuration promotes thermodynamically favorable asymmetric C–C coupling between *CO and *OCH<sub>2</sub>, forming the critical CO–OCH₂ intermediate and facilitating C<sub>2</sub>H<sub>5</sub>OH production, as opposed to symmetric O–Cu–O sites that mainly generate HCOOH. This work offers an effective strategy for designing multi-active-site catalysts toward highly selective CO₂ reduction to C<sub>2</sub>H<sub>5</sub>OH and provides fundamental insight into the reaction mechanism.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"37 1","pages":"Article 111926"},"PeriodicalIF":8.9,"publicationDate":"2025-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145463678","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 : 2025-09-30DOI: 10.1016/j.cclet.2025.111929
Ao Zhou , Mostafa M.K. Amer , Qin Yin
Asymmetric reduction of unsaturated compounds via dynamic kinetic resolution (DKR) has significantly enhanced the efficiency and selectivity of synthesizing enantiomerically pure compounds from racemic substrates. This approach combines the simultaneous racemization of substrates with enantioselective reduction, enabling quantitative yields and high enantiomeric excess. In the past several years, remarkable advances in this field have been achieved, ranging from the development of innovative catalytic systems, novel synthetic strategies, expansion of substrate scope, deeper mechanistic understanding, and their applications. These advancements offer alternative and efficient methods in the asymmetric synthesis of chiral molecules bearing multiple consecutive stereogenic centers, particularly beneficial for the synthesis of natural products or chiral intermediates in pharmaceuticals and fine chemicals. In this review, we summarize the recent advances during the last several years according to the substrate types in this powerful and productive field, with an emphasis on the development of new catalytic systems and the insight into the DKR process.
{"title":"Recent advances on asymmetric reduction via dynamic kinetic resolution","authors":"Ao Zhou , Mostafa M.K. Amer , Qin Yin","doi":"10.1016/j.cclet.2025.111929","DOIUrl":"10.1016/j.cclet.2025.111929","url":null,"abstract":"<div><div>Asymmetric reduction of unsaturated compounds <em>via</em> dynamic kinetic resolution (DKR) has significantly enhanced the efficiency and selectivity of synthesizing enantiomerically pure compounds from racemic substrates. This approach combines the simultaneous racemization of substrates with enantioselective reduction, enabling quantitative yields and high enantiomeric excess. In the past several years, remarkable advances in this field have been achieved, ranging from the development of innovative catalytic systems, novel synthetic strategies, expansion of substrate scope, deeper mechanistic understanding, and their applications. These advancements offer alternative and efficient methods in the asymmetric synthesis of chiral molecules bearing multiple consecutive stereogenic centers, particularly beneficial for the synthesis of natural products or chiral intermediates in pharmaceuticals and fine chemicals. In this review, we summarize the recent advances during the last several years according to the substrate types in this powerful and productive field, with an emphasis on the development of new catalytic systems and the insight into the DKR process.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"37 5","pages":"Article 111929"},"PeriodicalIF":8.9,"publicationDate":"2025-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146186613","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 : 2025-09-29DOI: 10.1016/j.cclet.2025.111905
Dongfan Li , Jinlong Lv , Jian-Cang Wang , Jiaxiang Liu , Huizhe Niu , Lu Yang , Hao Luo , Du Lv , Lichun Niu , Zemin He , Zongcheng Miao
The advent of all-solid-state lithium metal batteries (ASSLMBs) holds promise for overcoming the safety hazards and energy density limitations faced by traditional lithium-ion batteries, thereby advancing the industrialization of next-generation energy storage technologies with high safety and specific energy. However, during practical application, three core challenges persist at the interface between the solid-state electrolytes (SSEs) and the lithium metal anode (LMA): Poor physical contact, interfacial side reactions, and growth of lithium dendrites. These interfacial issues constrain the overall performance of ASSLMBs and impede the commercialization process of this battery system. This review begins by examining the underlying mechanisms responsible for the interfacial problems between SSEs and LMA. Building on this foundation, optimization strategies and recent research progress are systematically introduced, classified according to the interfacial components: SSE-side optimizations, interface engineering, and LMA-side treatments. Finally, future research directions, strategies, and optimization schemes addressing the interfacial challenges between SSEs and LMA are prospected. This analysis aims to facilitate critical breakthroughs in the stability, cycling lifespan, and energy density of ASSLMBs, promoting their transition from laboratory innovation to commercial application.
{"title":"Interface challenges of solid-state electrolytes/lithium metal anode: From origin analysis, failure mechanism to interface optimization strategies","authors":"Dongfan Li , Jinlong Lv , Jian-Cang Wang , Jiaxiang Liu , Huizhe Niu , Lu Yang , Hao Luo , Du Lv , Lichun Niu , Zemin He , Zongcheng Miao","doi":"10.1016/j.cclet.2025.111905","DOIUrl":"10.1016/j.cclet.2025.111905","url":null,"abstract":"<div><div>The advent of all-solid-state lithium metal batteries (ASSLMBs) holds promise for overcoming the safety hazards and energy density limitations faced by traditional lithium-ion batteries, thereby advancing the industrialization of next-generation energy storage technologies with high safety and specific energy. However, during practical application, three core challenges persist at the interface between the solid-state electrolytes (SSEs) and the lithium metal anode (LMA): Poor physical contact, interfacial side reactions, and growth of lithium dendrites. These interfacial issues constrain the overall performance of ASSLMBs and impede the commercialization process of this battery system. This review begins by examining the underlying mechanisms responsible for the interfacial problems between SSEs and LMA. Building on this foundation, optimization strategies and recent research progress are systematically introduced, classified according to the interfacial components: SSE-side optimizations, interface engineering, and LMA-side treatments. Finally, future research directions, strategies, and optimization schemes addressing the interfacial challenges between SSEs and LMA are prospected. This analysis aims to facilitate critical breakthroughs in the stability, cycling lifespan, and energy density of ASSLMBs, promoting their transition from laboratory innovation to commercial application.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"37 3","pages":"Article 111905"},"PeriodicalIF":8.9,"publicationDate":"2025-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145837504","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 : 2025-09-29DOI: 10.1016/j.cclet.2025.111917
Zhuojun Duan , Peiyue Jin , Houying Xing , Jian Chen , Yueting Yang , Yawen Tan , Song Liu
The hydrogen evolution reaction (HER) is crucial for hydrogen production and sustainable energy storage. Molybdenum disulfide (MoS2), a representative transition metal dichalcogenides (TMDs), shows potential as an HER catalyst but suffers from limited performance due to poor charge transfer and interfacial effects. Here, we report a salt-assisted chemical vapor deposition (CVD) method for synthesizing high-quality tungsten ditelluride (WTe2) with tunable morphologies using alkali halides (NaCl, KCl and LiCl). The prepared WTe2 nanoribbons and hexagonal nanosheets exhibit morphology-dependent electrical conductivity, with nanosheets showing superior performance. To evaluate WTe2 as a contact electrode, WTe2−MoS2 heterostructures were fabricated and compared with graphene-MoS2 counterparts. The WTe2−MoS2 heterostructure exhibits a superior Tafel slope of 111.57 mV/dec and an overpotential of 298 mV at -10 mA/cm2, significantly outperforming graphene-based electrodes. This improvement is attributed to the excellent conductivity of WTe2 and reduced interfacial Schottky barriers. Moreover, we systematically investigate the influence of WTe2 thickness on HER performance and assess the electrochemical durability and structural stability of the heterostructure, further confirming the effectiveness of WTe2 as a contact electrode for enhancing the HER activity of MoS2. This study offers a novel approach for enhancing the HER performance of MoS2 through controlled WTe2 growth and application as a contact electrode. Our findings provide valuable insights into the synthesis of high-quality WTe2 and broaden the potential applications of two-dimensional materials in energy catalysis.
{"title":"Salt-assisted synthesis of WTe2 contact electrodes for efficient MoS2-based hydrogen evolution reaction","authors":"Zhuojun Duan , Peiyue Jin , Houying Xing , Jian Chen , Yueting Yang , Yawen Tan , Song Liu","doi":"10.1016/j.cclet.2025.111917","DOIUrl":"10.1016/j.cclet.2025.111917","url":null,"abstract":"<div><div>The hydrogen evolution reaction (HER) is crucial for hydrogen production and sustainable energy storage. Molybdenum disulfide (MoS<sub>2</sub>), a representative transition metal dichalcogenides (TMDs), shows potential as an HER catalyst but suffers from limited performance due to poor charge transfer and interfacial effects. Here, we report a salt-assisted chemical vapor deposition (CVD) method for synthesizing high-quality tungsten ditelluride (WTe<sub>2</sub>) with tunable morphologies using alkali halides (NaCl, KCl and LiCl). The prepared WTe<sub>2</sub> nanoribbons and hexagonal nanosheets exhibit morphology-dependent electrical conductivity, with nanosheets showing superior performance. To evaluate WTe<sub>2</sub> as a contact electrode, WTe<sub>2</sub>−MoS<sub>2</sub> heterostructures were fabricated and compared with graphene-MoS<sub>2</sub> counterparts. The WTe<sub>2</sub>−MoS<sub>2</sub> heterostructure exhibits a superior Tafel slope of 111.57 mV/dec and an overpotential of 298 mV at -10 mA/cm<sup>2</sup>, significantly outperforming graphene-based electrodes. This improvement is attributed to the excellent conductivity of WTe<sub>2</sub> and reduced interfacial Schottky barriers. Moreover, we systematically investigate the influence of WTe<sub>2</sub> thickness on HER performance and assess the electrochemical durability and structural stability of the heterostructure, further confirming the effectiveness of WTe<sub>2</sub> as a contact electrode for enhancing the HER activity of MoS<sub>2</sub>. This study offers a novel approach for enhancing the HER performance of MoS<sub>2</sub> through controlled WTe<sub>2</sub> growth and application as a contact electrode. Our findings provide valuable insights into the synthesis of high-quality WTe<sub>2</sub> and broaden the potential applications of two-dimensional materials in energy catalysis.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"37 2","pages":"Article 111917"},"PeriodicalIF":8.9,"publicationDate":"2025-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145691098","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 : 2025-09-29DOI: 10.1016/j.cclet.2025.111916
Ruijing Fu , Bin Xiao , Haoyuan Weng , Pan Wang , Guangxia Wang , Qingguang Zeng , Dawei Wen , Guanjun Xiao
Luminescent materials function as optical pressure sensors based on pressure-dependent emission. Optical pressure sensors offer a broad measurement range and non-contact operation but face limitations in sensitivity. In this study, we establish a selection principle based on low-dimensional structures and conduct a high-pressure evaluation of xCr3+-doped Sr9Ga1-x(PO4)7 (x = 0.2, 0.5, and 0.8) phosphor, demonstrating its exceptional pressure sensitivity. Upon excitation at 488 nm, Sr9Ga0.5(PO4)7:0.5Cr3+ displays a broad near-infrared emission peak centered at 840 nm. Specifically, the phosphor maintains its structural integrity under pressures up to 10.0 GPa, with a continuous blue shift. The fluorescence peak shifts from 839.5 nm to 757.9 nm, demonstrating a high-pressure sensitivity of 8.11 nm/GPa. These findings establish Sr9Ga0.5(PO4)7:0.5Cr3+ as a viable candidate for optical pressure sensor, thereby offering valuable insights into advancing optical sensor development through host selection.
{"title":"An optical pressure sensing phosphor of high-sensitivity by soft structure","authors":"Ruijing Fu , Bin Xiao , Haoyuan Weng , Pan Wang , Guangxia Wang , Qingguang Zeng , Dawei Wen , Guanjun Xiao","doi":"10.1016/j.cclet.2025.111916","DOIUrl":"10.1016/j.cclet.2025.111916","url":null,"abstract":"<div><div>Luminescent materials function as optical pressure sensors based on pressure-dependent emission. Optical pressure sensors offer a broad measurement range and non-contact operation but face limitations in sensitivity. In this study, we establish a selection principle based on low-dimensional structures and conduct a high-pressure evaluation of <em>x</em>Cr<sup>3+</sup>-doped Sr<sub>9</sub>Ga<sub>1-</sub><em><sub>x</sub></em>(PO<sub>4</sub>)<sub>7</sub> (<em>x</em> = 0.2, 0.5, and 0.8) phosphor, demonstrating its exceptional pressure sensitivity. Upon excitation at 488 nm, Sr<sub>9</sub>Ga<sub>0.5</sub>(PO<sub>4</sub>)<sub>7</sub>:0.5Cr<sup>3+</sup> displays a broad near-infrared emission peak centered at 840 nm. Specifically, the phosphor maintains its structural integrity under pressures up to 10.0 GPa, with a continuous blue shift. The fluorescence peak shifts from 839.5 nm to 757.9 nm, demonstrating a high-pressure sensitivity of 8.11 nm/GPa. These findings establish Sr<sub>9</sub>Ga<sub>0.5</sub>(PO<sub>4</sub>)<sub>7</sub>:0.5Cr<sup>3+</sup> as a viable candidate for optical pressure sensor, thereby offering valuable insights into advancing optical sensor development through host selection.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"37 3","pages":"Article 111916"},"PeriodicalIF":8.9,"publicationDate":"2025-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145788334","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 : 2025-09-29DOI: 10.1016/j.cclet.2025.111925
Dongfang Liu , Zhouyu Wang , Junli Wang , Leyong Wang
{"title":"The 5th Xihua Chemistry and Biomedicine Forum","authors":"Dongfang Liu , Zhouyu Wang , Junli Wang , Leyong Wang","doi":"10.1016/j.cclet.2025.111925","DOIUrl":"10.1016/j.cclet.2025.111925","url":null,"abstract":"","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"37 2","pages":"Article 111925"},"PeriodicalIF":8.9,"publicationDate":"2025-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145578506","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 : 2025-09-29DOI: 10.1016/j.cclet.2025.111920
Lihui Ou , Zhancheng Liu , Dai-Huo Liu , Zhi Zhang
Cu electrocatalysts have been demonstrated to have unique ability to reduce CO2 to various high value-added C2 products like ethylene and alcohols. However, realizing high selectivity of C2 products are still a main challenge due to complex CO2 electroreduction pathways and small opportunity of CC coupling reactions. Here, we found the origin of enhanced CO2 electroreduction reaction activity and product selectivity towards C2 products and CC coupling mechanism at halogen atoms-adsorbed Cu/H2O interfaces, the corresponding CO2 electroreduction evolution mechanisms at the halogen atoms-modified Cu/H2O interfaces are systematically studied via theoretical modeling and calculations. The calculated results indicate that halide anions modifications are beneficial to CO dimerization into OCCO dimer, especially Cl−-adsorbed Cu(111)/H2O interface has the optimum activity and selectivity towards OCCO dimer, subsequent Cl-adsorbed Cu(111)/H2O interface can selectively reduce CO2 into C2H4 product. The function relationship between adsorption free energy of Cl atom and electrode potential explain why the adsorption of Cl− can enhance selectivity of C2H4 product. The determinations of onset potentials indicate that electroreduction pathways of CO2 towards C2H4 product are facile to take place and further explain the origin of the significantly enhanced CO production activity and C2H4 product selectivity. This work on selective realization of CO2 electroreduction towards C2H4 product via Cl−-modified Cu(111)/H2O interface provide a theoretical guideline for how to selectively realize other high value-added C2 products.
{"title":"Cl-adsorbed Cu(111)/H2O interface selectively realizes electrochemical CO2 reduction towards C2H4 product: Mechanistic understanding","authors":"Lihui Ou , Zhancheng Liu , Dai-Huo Liu , Zhi Zhang","doi":"10.1016/j.cclet.2025.111920","DOIUrl":"10.1016/j.cclet.2025.111920","url":null,"abstract":"<div><div>Cu electrocatalysts have been demonstrated to have unique ability to reduce CO<sub>2</sub> to various high value-added C<sub>2</sub> products like ethylene and alcohols. However, realizing high selectivity of C<sub>2</sub> products are still a main challenge due to complex CO<sub>2</sub> electroreduction pathways and small opportunity of C<img>C coupling reactions. Here, we found the origin of enhanced CO<sub>2</sub> electroreduction reaction activity and product selectivity towards C<sub>2</sub> products and C<img>C coupling mechanism at halogen atoms-adsorbed Cu/H<sub>2</sub>O interfaces, the corresponding CO<sub>2</sub> electroreduction evolution mechanisms at the halogen atoms-modified Cu/H<sub>2</sub>O interfaces are systematically studied <em>via</em> theoretical modeling and calculations. The calculated results indicate that halide anions modifications are beneficial to CO dimerization into OCCO dimer, especially Cl<sup>−</sup>-adsorbed Cu(111)/H<sub>2</sub>O interface has the optimum activity and selectivity towards OCCO dimer, subsequent Cl-adsorbed Cu(111)/H<sub>2</sub>O interface can selectively reduce CO<sub>2</sub> into C<sub>2</sub>H<sub>4</sub> product. The function relationship between adsorption free energy of Cl atom and electrode potential explain why the adsorption of Cl<sup>−</sup> can enhance selectivity of C<sub>2</sub>H<sub>4</sub> product. The determinations of onset potentials indicate that electroreduction pathways of CO<sub>2</sub> towards C<sub>2</sub>H<sub>4</sub> product are facile to take place and further explain the origin of the significantly enhanced CO production activity and C<sub>2</sub>H<sub>4</sub> product selectivity. This work on selective realization of CO<sub>2</sub> electroreduction towards C<sub>2</sub>H<sub>4</sub> product <em>via</em> Cl<sup>−</sup>-modified Cu(111)/H<sub>2</sub>O interface provide a theoretical guideline for how to selectively realize other high value-added C<sub>2</sub> products.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"37 2","pages":"Article 111920"},"PeriodicalIF":8.9,"publicationDate":"2025-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145622080","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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