Pub Date : 2026-02-01Epub Date: 2025-09-25DOI: 10.1016/j.cjsc.2025.100748
Chao Ma, Jian Li
{"title":"Expediting the discovery of extra-large-pore zeolites enabled by MicroED and combinatorial chemistry","authors":"Chao Ma, Jian Li","doi":"10.1016/j.cjsc.2025.100748","DOIUrl":"10.1016/j.cjsc.2025.100748","url":null,"abstract":"","PeriodicalId":10151,"journal":{"name":"结构化学","volume":"45 2","pages":"Article 100748"},"PeriodicalIF":10.3,"publicationDate":"2026-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146147414","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-02-01Epub Date: 2025-10-22DOI: 10.1016/j.cjsc.2025.100770
Weilin Kong , Man Lian , Tong Sheng , Yarui Wang , Lu Zou , Kaisheng Xia , Jian Pu , Bo Chi , Yunfeng Tian
Nanofibers hold great promise as oxygen electrode materials in solid oxide cells (SOCs). However, conventional fabrication methods—such as slurry processing and high-temperature sintering—inevitably disrupt their delicate nano-architectures. Here, we propose an innovative self-assembly strategy mediated by current polarization to construct La0.6Sr0.4Co0.2Fe0.8O3−δ-Gd0.1Ce0.9O2−δ (LSCF-GDC) nanofiber composite film electrodes. This approach largely preserves the fibrous morphology while promoting coherent heterointerfaces, abundant active sites, and efficient electron/ion pathways. Benefiting from this tailored architecture, the electrode achieves a low polarization resistance of 0.117 Ω cm2 and a peak power density of 1.482 W cm−2 at 800 °C. Moreover, in CO2 electrolysis mode, it delivers an impressive current density of 2.30 A cm−2 at 1.8 V. These results establish nanofiber heterostructure films, enabled by current polarization assembly, as a powerful strategy to simultaneously enhance activity, durability, and mass transport, offering new opportunities for high-performance intermediate-temperature SOCs.
纳米纤维在固体氧化物电池（soc）中作为氧电极材料具有广阔的应用前景。然而，传统的制造方法——如浆液处理和高温烧结——不可避免地破坏了它们精致的纳米结构。在此，我们提出了一种创新的电流极化自组装策略，构建La0.6Sr0.4Co0.2Fe0.8O3−δ- gd0.1 ce0.9 o2−δ (LSCF-GDC)纳米纤维复合膜电极。这种方法在很大程度上保留了纤维形态，同时促进了相干异质界面、丰富的活性位点和高效的电子/离子通路。得益于这种定制的结构，该电极在800°C时实现了0.117 Ω cm2的低极化电阻和1.482 W cm−2的峰值功率密度。此外，在CO2电解模式下，它在1.8 V下提供了令人印象深刻的2.30 A cm - 2电流密度。这些结果建立了纳米纤维异质结构薄膜，通过电流极化组装，作为同时增强活性，耐久性和质量传输的强大策略，为高性能中温soc提供了新的机会。
{"title":"Unidimensional heterostructured LSCF-GDC nanofiber film as oxygen electrode for efficient solid oxide cell","authors":"Weilin Kong , Man Lian , Tong Sheng , Yarui Wang , Lu Zou , Kaisheng Xia , Jian Pu , Bo Chi , Yunfeng Tian","doi":"10.1016/j.cjsc.2025.100770","DOIUrl":"10.1016/j.cjsc.2025.100770","url":null,"abstract":"<div><div>Nanofibers hold great promise as oxygen electrode materials in solid oxide cells (SOCs). However, conventional fabrication methods—such as slurry processing and high-temperature sintering—inevitably disrupt their delicate nano-architectures. Here, we propose an innovative self-assembly strategy mediated by current polarization to construct La<sub>0.6</sub>Sr<sub>0.4</sub>Co<sub>0.2</sub>Fe<sub>0.8</sub>O<sub>3</sub><sub>−</sub><sub><em>δ</em></sub>-Gd<sub>0.1</sub>Ce<sub>0.9</sub>O<sub>2</sub><sub>−</sub><sub><em>δ</em></sub> (LSCF-GDC) nanofiber composite film electrodes. This approach largely preserves the fibrous morphology while promoting coherent heterointerfaces, abundant active sites, and efficient electron/ion pathways. Benefiting from this tailored architecture, the electrode achieves a low polarization resistance of 0.117 Ω cm<sup>2</sup> and a peak power density of 1.482 W cm<sup>−2</sup> at 800 °C. Moreover, in CO<sub>2</sub> electrolysis mode, it delivers an impressive current density of 2.30 A cm<sup>−2</sup> at 1.8 V. These results establish nanofiber heterostructure films, enabled by current polarization assembly, as a powerful strategy to simultaneously enhance activity, durability, and mass transport, offering new opportunities for high-performance intermediate-temperature SOCs.</div></div>","PeriodicalId":10151,"journal":{"name":"结构化学","volume":"45 2","pages":"Article 100770"},"PeriodicalIF":10.3,"publicationDate":"2026-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146147639","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-02-01Epub Date: 2025-10-25DOI: 10.1016/j.cjsc.2025.100791
Baker Rhimi , Zheyang Liu , Jing Li , Min Zhou , Qiang Ma , Zhifeng Jiang
Diatomic-site catalysts (DACs) have recently emerged as highly promising platforms for photocatalytic CO2 reduction, offering unique opportunities to control reaction thermodynamics and kinetics for selective C2+ product formation. By integrating two adjacent metal centers within well-defined architectures, DACs enable synergistic activation of CO2 and stabilization of key C–C coupling intermediates, surpassing the limitations of single-atom or bulk catalysts. This perspective highlights the recent advances in DAC synthesis strategies, characterization techniques, mechanistic insights into multi-carbon formation, and the fundamental reasons why DACs facilitate C–C bond formation with high selectivity. A critical discussion is presented on the mechanism of C2+ formation on these unique active sites. Furthermore, the role of defect engineering within the catalyst support or surrounding matrix in modulating the electronic structure and stability of DACs is thoroughly examined. Finally, this perspective outlines future research directions to further unlock the full potential of DACs for efficient and selective photocatalytic CO2 reduction to C2+ products.
{"title":"The potential of diatomic-site catalysts for CO2 photoreduction to multi-carbon products","authors":"Baker Rhimi , Zheyang Liu , Jing Li , Min Zhou , Qiang Ma , Zhifeng Jiang","doi":"10.1016/j.cjsc.2025.100791","DOIUrl":"10.1016/j.cjsc.2025.100791","url":null,"abstract":"<div><div>Diatomic-site catalysts (DACs) have recently emerged as highly promising platforms for photocatalytic CO<sub>2</sub> reduction, offering unique opportunities to control reaction thermodynamics and kinetics for selective C<sub>2+</sub> product formation. By integrating two adjacent metal centers within well-defined architectures, DACs enable synergistic activation of CO<sub>2</sub> and stabilization of key C–C coupling intermediates, surpassing the limitations of single-atom or bulk catalysts. This perspective highlights the recent advances in DAC synthesis strategies, characterization techniques, mechanistic insights into multi-carbon formation, and the fundamental reasons why DACs facilitate C–C bond formation with high selectivity. A critical discussion is presented on the mechanism of C<sub>2+</sub> formation on these unique active sites. Furthermore, the role of defect engineering within the catalyst support or surrounding matrix in modulating the electronic structure and stability of DACs is thoroughly examined. Finally, this perspective outlines future research directions to further unlock the full potential of DACs for efficient and selective photocatalytic CO<sub>2</sub> reduction to C<sub>2+</sub> products.</div></div>","PeriodicalId":10151,"journal":{"name":"结构化学","volume":"45 2","pages":"Article 100791"},"PeriodicalIF":10.3,"publicationDate":"2026-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146147632","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-01Epub Date: 2025-10-16DOI: 10.1016/j.cjsc.2025.100769
Yi Li, Ye Lu, Shi-Ping Yang
Coordination-directed synthesis has emerged as an effective and versatile approach for constructing mechanically interlocked molecules (MIMs). This field has long been dominated by Werner-type complexes featuring oxygen and/or nitrogen donors, whereas assemblies incorporating N-heterocyclic carbene (NHC) donors remain underexplored. This review provides a comprehensive overview of the rapidly developing field of MIMs constructed from poly-NHC-based building blocks. By highlighting representative recent examples, this review focuses on the pivotal role of NHC ligands and the robustness of metal-CNHC bond in the construction of metallosupramolecular interlocked structures. In addition, it summarizes contemporary strategies for achieving efficient assembly, analyzes defining structural attributes of the resulting architectures, and outlines current challenges and emerging opportunities for future developments in NHC-based MIMs.
{"title":"Organometallic mechanically interlocked molecules featuring N-heterocyclic carbene ligands: Recent advances in synthesis and applications","authors":"Yi Li, Ye Lu, Shi-Ping Yang","doi":"10.1016/j.cjsc.2025.100769","DOIUrl":"10.1016/j.cjsc.2025.100769","url":null,"abstract":"<div><div>Coordination-directed synthesis has emerged as an effective and versatile approach for constructing mechanically interlocked molecules (MIMs). This field has long been dominated by Werner-type complexes featuring oxygen and/or nitrogen donors, whereas assemblies incorporating N-heterocyclic carbene (NHC) donors remain underexplored. This review provides a comprehensive overview of the rapidly developing field of MIMs constructed from poly-NHC-based building blocks. By highlighting representative recent examples, this review focuses on the pivotal role of NHC ligands and the robustness of metal-C<sub>NHC</sub> bond in the construction of metallosupramolecular interlocked structures. In addition, it summarizes contemporary strategies for achieving efficient assembly, analyzes defining structural attributes of the resulting architectures, and outlines current challenges and emerging opportunities for future developments in NHC-based MIMs.</div></div>","PeriodicalId":10151,"journal":{"name":"结构化学","volume":"45 1","pages":"Article 100769"},"PeriodicalIF":10.3,"publicationDate":"2026-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145941444","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Covalent organic frameworks (COFs), as a burgeoning type of porous material, have attracted significant attention due to their intriguing structural characteristics and customizable functionalities. Particularly, COFs that exhibit luminescent properties have garnered significant attention in fields like chemical sensing, biosensing, photocatalysis, optoelectronics applications and so on. This article systematically examines the synthetic strategies for luminescent covalent organic frameworks (LCOFs) and provides a comprehensive summary based on linkage-type classification. It further provides a comprehensive summary and emphasizes the broad and notable applications of LCOFs across multiple areas, such as luminescent applications, circularly polarized luminescence, fluorescent imaging, biomedicine, and chemical and biological sensing. Finally, the primary challenges and future directions of LCOFs concerning their synthetic method, structural design and optical properties are discussed. This review helps researchers quickly understand the current research status in this field, and points out the direction for subsequent related research work. It is expected to promote the further development and application expansion of LCOFs synthesis technology, which has important academic value.
{"title":"Luminescent covalent organic frameworks: Classification to optical applications","authors":"Yu-Qin Xia , Shui-Ming Jing , Li-Mei Chang , Zhi-Gang Gu , Jian Zhang","doi":"10.1016/j.cjsc.2025.100731","DOIUrl":"10.1016/j.cjsc.2025.100731","url":null,"abstract":"<div><div>Covalent organic frameworks (COFs), as a burgeoning type of porous material, have attracted significant attention due to their intriguing structural characteristics and customizable functionalities. Particularly, COFs that exhibit luminescent properties have garnered significant attention in fields like chemical sensing, biosensing, photocatalysis, optoelectronics applications and so on. This article systematically examines the synthetic strategies for luminescent covalent organic frameworks (LCOFs) and provides a comprehensive summary based on linkage-type classification. It further provides a comprehensive summary and emphasizes the broad and notable applications of LCOFs across multiple areas, such as luminescent applications, circularly polarized luminescence, fluorescent imaging, biomedicine, and chemical and biological sensing. Finally, the primary challenges and future directions of LCOFs concerning their synthetic method, structural design and optical properties are discussed. This review helps researchers quickly understand the current research status in this field, and points out the direction for subsequent related research work. It is expected to promote the further development and application expansion of LCOFs synthesis technology, which has important academic value.</div></div>","PeriodicalId":10151,"journal":{"name":"结构化学","volume":"45 1","pages":"Article 100731"},"PeriodicalIF":10.3,"publicationDate":"2026-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145941445","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-01Epub Date: 2025-10-11DOI: 10.1016/j.cjsc.2025.100764
Ya-Xuan Xue , Han Xu , Jia-Nan Chen , Hai-Quan Tian , Tao Jia , Wei-Dong Liu , Chong-Yang Li , La-Sheng Long , Lan-Sun Zheng , Xiang-Jian Kong
Heterometallic 3d-4f clusters represent a promising class of multifunctional molecular materials, driven by the synergistic interactions between d- and f-electrons. Incorporating chirality into these systems further expands their potential applications, particularly in chiroptical and magneto-optical technologies. Herein, we report the successful synthesis of chiral [Ln3Co5] (Ln = Er and Y) clusters using binaphthol-based ligands. Single-crystal X-ray diffraction reveals the coexistence of two distinct Co2+ coordination geometries: six-coordinate octahedron and five-coordinate trigonal bipyramid. Spectroscopic analyses demonstrate geometry-dependent chiroptical behavior: pentacoordinate Co2+ ions predominantly contribute to the circular dichroism (CD) features, while both geometries exhibit distinguishable signals in the magnetic circular dichroism (MCD) spectra. Notably, a pronounced magnetic dipole transition (4I15/2 → 4I13/2) from Er3+ centers is observed in the near-infrared MCD region, displaying a high g-factor of 0.0078 T−1. This work highlights the configuration- and ligand field-dependent chiroptical responses in 3d-4f systems, providing new insights for the rational design of advanced magneto-optical devices.
{"title":"Chiral Ln3Co5 clusters with geometry-dependent chiroptical and magneto-optical properties","authors":"Ya-Xuan Xue , Han Xu , Jia-Nan Chen , Hai-Quan Tian , Tao Jia , Wei-Dong Liu , Chong-Yang Li , La-Sheng Long , Lan-Sun Zheng , Xiang-Jian Kong","doi":"10.1016/j.cjsc.2025.100764","DOIUrl":"10.1016/j.cjsc.2025.100764","url":null,"abstract":"<div><div>Heterometallic 3d-4f clusters represent a promising class of multifunctional molecular materials, driven by the synergistic interactions between d- and f-electrons. Incorporating chirality into these systems further expands their potential applications, particularly in chiroptical and magneto-optical technologies. Herein, we report the successful synthesis of chiral [Ln<sub>3</sub>Co<sub>5</sub>] (Ln = Er and Y) clusters using binaphthol-based ligands. Single-crystal X-ray diffraction reveals the coexistence of two distinct Co<sup>2+</sup> coordination geometries: six-coordinate octahedron and five-coordinate trigonal bipyramid. Spectroscopic analyses demonstrate geometry-dependent chiroptical behavior: pentacoordinate Co<sup>2+</sup> ions predominantly contribute to the circular dichroism (CD) features, while both geometries exhibit distinguishable signals in the magnetic circular dichroism (MCD) spectra. Notably, a pronounced magnetic dipole transition (<sup>4</sup>I<sub>15/2</sub> → <sup>4</sup>I<sub>13/2</sub>) from Er<sup>3+</sup> centers is observed in the near-infrared MCD region, displaying a high g-factor of 0.0078 T<sup>−</sup><sup>1</sup>. This work highlights the configuration- and ligand field-dependent chiroptical responses in 3d-4f systems, providing new insights for the rational design of advanced magneto-optical devices.</div></div>","PeriodicalId":10151,"journal":{"name":"结构化学","volume":"45 1","pages":"Article 100764"},"PeriodicalIF":10.3,"publicationDate":"2026-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145941519","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-01Epub Date: 2025-10-13DOI: 10.1016/j.cjsc.2025.100768
Lao-Bang Wang , Yaoyao Peng , Yu Fang , Jian-Ping Lang
Metal sulfide-bridged clusters exhibit unique topologies and functional properties, offering potential for advanced materials and biomimetic systems. However, challenges persist in their controlled synthesis, particularly in precise sulfide incorporation and structural modulation to form high-nuclearity clusters. Herein, we report an insitu molecular tailoring strategy using protonation of the [Tp∗WS3]− synthon by NH4+ to gradually release S2− ions, which react with in situ formed fragments such as [Tp∗WS3Cu3]2+ and [Tp∗WS3Cu2]+. Under the cooperative influence of Cl−, CN−, or Cu+, three low-nuclearity clusters with complex polyhedral structures are assembled. Solvent-induced post-scissoring and reassembly of these precursors afford two unprecedented high-nuclearity clusters with novel topological frameworks. Thin films derived from single crystals of all five clusters display significantly enhanced third-order nonlinear optical (NLO) responses compared to their solution-state counterparts. Importantly, the high-nuclearity clusters display NLO responses, surpassing not only those of their precursors but also the additive contributions of the individual units. Density functional theory (DFT) calculations attribute this enhancement to improved intracluster charge separation and synergistic interactions via linkers. This work establishes a versatile platform for constructing high-nuclearity metal sulfide clusters and provides new insights into designing functional analogues of nitrogenase-active sites.
{"title":"Molecular tailoring strategies for the controlled assembly of high-nuclearity sulfide-bridged metal clusters","authors":"Lao-Bang Wang , Yaoyao Peng , Yu Fang , Jian-Ping Lang","doi":"10.1016/j.cjsc.2025.100768","DOIUrl":"10.1016/j.cjsc.2025.100768","url":null,"abstract":"<div><div>Metal sulfide-bridged clusters exhibit unique topologies and functional properties, offering potential for advanced materials and biomimetic systems. However, challenges persist in their controlled synthesis, particularly in precise sulfide incorporation and structural modulation to form high-nuclearity clusters. Herein, we report an <em>in</em> <em>situ</em> molecular tailoring strategy using protonation of the [Tp<sup>∗</sup>WS<sub>3</sub>]<sup>−</sup> synthon by NH<sub>4</sub><sup>+</sup> to gradually release S<sup>2−</sup> ions, which react with <em>in situ</em> formed fragments such as [Tp<sup>∗</sup>WS<sub>3</sub>Cu<sub>3</sub>]<sup>2+</sup> and [Tp<sup>∗</sup>WS<sub>3</sub>Cu<sub>2</sub>]<sup>+</sup>. Under the cooperative influence of Cl<sup>−</sup>, CN<sup>−</sup>, or Cu<sup>+</sup>, three low-nuclearity clusters with complex polyhedral structures are assembled. Solvent-induced post-scissoring and reassembly of these precursors afford two unprecedented high-nuclearity clusters with novel topological frameworks. Thin films derived from single crystals of all five clusters display significantly enhanced third-order nonlinear optical (NLO) responses compared to their solution-state counterparts. Importantly, the high-nuclearity clusters display NLO responses, surpassing not only those of their precursors but also the additive contributions of the individual units. Density functional theory (DFT) calculations attribute this enhancement to improved intracluster charge separation and synergistic interactions via linkers. This work establishes a versatile platform for constructing high-nuclearity metal sulfide clusters and provides new insights into designing functional analogues of nitrogenase-active sites.</div></div>","PeriodicalId":10151,"journal":{"name":"结构化学","volume":"45 1","pages":"Article 100768"},"PeriodicalIF":10.3,"publicationDate":"2026-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145941516","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-01Epub Date: 2025-10-11DOI: 10.1016/j.cjsc.2025.100762
Dongdong Liu , Ziqi Tang , Haoyu Wang , Xinjie Li , Jingyang Li , Chao Zhu , Shan Ding , Yuan-Sheng Cheng , Hui Zhang , Peipei Li , Ju Wu , Guozan Yuan
Using solar energy to convert CO2 into chemicals presents an economical, environmentally friendly, and sustainable approach. However, single-component photocatalysts exhibit limitations, including a narrow light absorption range, rapid carrier recombination, and weak reduction capabilities. To mitigate charge carrier recombination and enhance reduction efficiency, this study prepared heterojunction photocatalysts by in situ growing zinc indium sulfide (ZnIn2S4) on a covalent organic framework (COF) substrate. Under visible light irradiation, the 30% ZIS-COF heterojunction demonstrated the highest CO2 reduction performance (1187.2 μmol g−1) and selectivity exceeding 99%, outperforming the single-component system. The electron transfer mechanism and catalytic process were further explored through photoluminescence (PL), time-resolved fluorescence decay spectra, attenuated total reflection Fourier transform infrared spectroscopy, and spin polarized density functional theory (DFT) calculations. The results reveal that, upon photoexcitation, electrons in COF migrate to ZnIn2S4 (ZIS), and the efficient flow of photoexcited electrons is facilitated by the intimate interface contact between COF and ZIS. Moreover, the porous structure of COF promotes CO2 adsorption and enhances mass transfer. This study establishes a versatile platform for developing various hybrid combinations of CO2-reducing metal semiconductors and photosensitizing COF materials, paving the way for enhanced photocatalytic performance.
{"title":"Rational design of ZnIn2S4–COF heterojunction to inhibit photogenerated carrier dynamics for enhanced photocatalytic CO2 reduction","authors":"Dongdong Liu , Ziqi Tang , Haoyu Wang , Xinjie Li , Jingyang Li , Chao Zhu , Shan Ding , Yuan-Sheng Cheng , Hui Zhang , Peipei Li , Ju Wu , Guozan Yuan","doi":"10.1016/j.cjsc.2025.100762","DOIUrl":"10.1016/j.cjsc.2025.100762","url":null,"abstract":"<div><div>Using solar energy to convert CO<sub>2</sub> into chemicals presents an economical, environmentally friendly, and sustainable approach. However, single-component photocatalysts exhibit limitations, including a narrow light absorption range, rapid carrier recombination, and weak reduction capabilities. To mitigate charge carrier recombination and enhance reduction efficiency, this study prepared heterojunction photocatalysts by <em>in situ</em> growing zinc indium sulfide (ZnIn<sub>2</sub>S<sub>4</sub>) on a covalent organic framework (COF) substrate. Under visible light irradiation, the 30% ZIS-COF heterojunction demonstrated the highest CO<sub>2</sub> reduction performance (1187.2 μmol g<sup>−1</sup>) and selectivity exceeding 99%, outperforming the single-component system. The electron transfer mechanism and catalytic process were further explored through photoluminescence (PL), time-resolved fluorescence decay spectra, attenuated total reflection Fourier transform infrared spectroscopy, and spin polarized density functional theory (DFT) calculations. The results reveal that, upon photoexcitation, electrons in COF migrate to ZnIn<sub>2</sub>S<sub>4</sub> (ZIS), and the efficient flow of photoexcited electrons is facilitated by the intimate interface contact between COF and ZIS. Moreover, the porous structure of COF promotes CO<sub>2</sub> adsorption and enhances mass transfer. This study establishes a versatile platform for developing various hybrid combinations of CO<sub>2</sub>-reducing metal semiconductors and photosensitizing COF materials, paving the way for enhanced photocatalytic performance.</div></div>","PeriodicalId":10151,"journal":{"name":"结构化学","volume":"45 1","pages":"Article 100762"},"PeriodicalIF":10.3,"publicationDate":"2026-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145941142","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-01Epub Date: 2025-10-09DOI: 10.1016/j.cjsc.2025.100760
Yiming Jin , Mingming Pan , Wei Luo
Addressing the CO-sensitive and catalytic efficiency issues of noble metal-based electrocatalysts towards alkaline hydrogen oxidation reaction (HOR) is indispensable for the practical commercialization of advanced anion exchange membrane fuel cells (AEMFCs). Here, Ni–N–C supported Ir catalysts denoted as Ir/Ni–N–C have been constructed and demonstrated greatly improved resistance towards CO impurities compared to conventional N–C or pure C anchored Ir nanoparticles after long-term CO poisoning. Besides, Ir/Ni–N–C possesses superior specific and mass activity of 0.557 mA cm−2 and 1.15 mA μgPGM−1, which is approximately 2-times higher than that of Ir/C and even outperforms the state-of-the-art commercial Pt/C catalysts. Combining in-situ surface-enhanced infrared absorption spectroscopy and density functional calculation, the band structure modulation and coordination effect of Ni–N–C supports lead to strengthened hydroxyl binding energy, promoted CO oxidative desorption under working potential, and lowered activation barrier of the rate-determining process of alkaline HOR. This work sheds light on the importance of metal–N–C substrates for solving the CO-tolerance and intrinsic activity challenges, and provides new insights for noble-metal based catalysts designing.
解决贵金属基电催化剂对碱性氢氧化反应（HOR）的co敏感性和催化效率问题是先进阴离子交换膜燃料电池（aemfc）实际商业化的必要条件。本文构建了Ni-N-C负载的Ir催化剂，表示为Ir/ Ni-N-C，与传统的N-C或纯C锚定的Ir纳米颗粒相比，在长期CO中毒后，它们对CO杂质的抵抗力大大提高。Ir/ Ni-N-C催化剂的比活性和质量活性分别为0.557 mA cm−2和1.15 mA μgPGM−1，比Ir/C催化剂高约2倍，甚至优于目前最先进的商业Pt/C催化剂。结合原位表面增强红外吸收光谱和密度泛函计算，发现Ni-N-C载体的能带结构调制和配位效应增强了羟基结合能，促进了CO在工作电位下的氧化解吸，降低了碱性HOR定速过程的激活势垒。这项工作揭示了金属- n - c底物对解决co耐受性和内在活性挑战的重要性，并为贵金属基催化剂的设计提供了新的见解。
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