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Efficient photocatalytic reduction of CO2 to formate by a molecular noble metal-free system

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Science China chemistry 2025年第1期68卷 152-156页

作者： Lihua Zhang Lingjing Chen Huatian Shi Yue Wei Gui Chen Tai-Chu Lau School of Environment and Civil Engineering Research Center for Eco-environmental Engineering Dongguan University of Technology Department of chemistry and Institute of Molecular Functional Materials City University of Hong Kong

Reducing CO2to carbon-neutral solar fuels can not only alleviate the energy demand but also mitigate the greenhouse *** present,developing an efficient non-noble metal photo/electrocatalytic system for converting CO2to a specific product beyond CO is still a big ***,we report a new cobalt complex bearing 2,2′-bi-1,10-phenanthroline ligand that can photocatalytically reduce CO2to formate （HCOO-）.Turnover number （TON） for HCOO-up to 677 with 99%selectivity can be achieved using organic dyes purpurin as photosensitizer and 1,3-dimethyl-2-phenyl-2,3-dihydro-1H-benzo[d]imidazole （BIH） as sacrificial reductant in a CO2-saturated NMP/TEA （v/v,3:1） solution under visible light *** potential electrolysis at-1.41 V （***/Ag Cl） in the presence of 12 m M Et3NHBF4also produced HCOO-with Faradaic efficiency of 39%.Spectroscopic and electrochemical studies suggest that a[CoI-H]species is the key intermediate for CO2reduction.

关键词： photocatalysis noble metal-free CO2 reduction formate cobalt hydride

An internally linked dibenzihexaphyrin

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Science China chemistry 2025年

作者： Zhaohui Zong Xiaotong Zhang Zhe Liu Guangliu Ran Wenkai Zhang Xiansheng Ke College of chemistry Beijing Normal University School of Physics and Astronomy Applied Optics Beijing Area Major Laboratory Center for Advanced Quantum Studies Beijing Normal University Key Laboratory of Multiscale Spin Physics Ministry of Education Beijing Normal University

Hexaphyrins are one of the most studied expanded porphyrins that show intriguing electronic structure and coordination abilities in the past decades. However, core-modified hexaphyrins especially for benzene-replaced hexaphyrins are much less ***, we revisit the dibenzihexaphyrin system and demonstrate how to achieve the hexaphyrin-like organometallic nature of a benzene-replaced expanded porphyrin. For the “true” di-m-benzihexaphyrin 2, metal complex with anticipated CCNN coordination is not realized probably due to the steric hindrance. Further, we synthesized an internally linked dibenzihexaphyrin (3)with a direct carbon–carbon bond between two phenylenes. As prepared, 3 has a strained biphenyl unit and can effectively coordinate two Cu(III) ions with CCNN coordination. This sharp contrast underscores the critical importance of the formed preorganized corrole-like adj-CCNN cavities after linking two flanking phenylenes. 3 can also act as a bidentate ligand like traditional hexaphyrin, enabling the formation of an even more strained bis-Rh(I) complex. The electronic structures and photophysical properties of the free base and metal complexes are systematically studied by steady state absorption and fstransient absorptions (fs-TA) spectroscopies, as well as DFTcalculations. Notably, 3 can be regarded as a hexaphyrin-sized backto-back fused bis-dicarbacorrole, which stands as the smallest fused carbaporphyrinoid array prepared to date.

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Enantioselective β-alkenylation of α,β-unsaturated aldehydes via chiral biphosphine ligand modified dirhodium(II) catalysis

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Science China chemistry 2025年

作者： Guangli Xu Hongda Chen Xiaoming Wang State Key Laboratory of Organometallic chemistry and Shanghai Hongkong Joint Laboratory in Chemical Synthesis Center for Excellence in Molecular Synthesis Shanghai Institute of Organic Chemistry University of Chinese Academy of Sciences Chinese Academy of Sciences School of chemistry and Materials Science Hangzhou Institute for Advanced Study University of Chinese Academy of Sciences School of chemistry and Chemical Engineering Henan Normal University

Dirhodium(II) complexes have achieved great success in organic synthesis,and fine-tuning their catalytic properties with various bridging ligands is well-investigated in carbene ***,combining dirhodium(II) with a sophisticated ligand as a catalyst in other reactions is still extremely challenging,especially for the asymmetric synthesis of valuable chiral ***,we report a dirhodium(II)/(S)-MeO-BIPHEP catalytic system for the challenging asymmetric β-alkenylation of α,β-unsaturated aldehydes,affording the corresponding chiral conjugate addition products in good yields with high enantioselectivities.A couple of drug-derived substrates were also compatible with the protocol,which has been successfully used to prepare biologically relevant pyranochromene *** mechanistic studies suggested that the dirhodium core might remain intact over the catalytic cycle,and the chiral diphosphine ligand plays a key role in this novel reactivity and determining the high enantioselectivities of the asymmetric conjugate addition.

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Unraveling the impacts of intermolecular interaction on morphology evolution for highly efficient organic solar cells and modules

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Science China chemistry 2025年第1期68卷 264-272页

作者： Xueqing Ma Yingying Cheng Yuqiang Liu Xinming Zheng Guangliu Ran Hongxiang Li Xinyue Cui Andong Zhang Wenkai Zhang Pei Cheng Wenchao Huang Zhishan Bo Beijing Key Laboratory of Energy Conversion and Storage Materials College of Chemistry Beijing Normal University College of Textiles and Clothing State Key Laboratory of Bio-fibers and Eco-textiles Qingdao University Key State Laboratory of Advanced Technology for Materials Synthesis and Processing School of Materials Science and EngineeringWuhan University of Technology Department of Physics and Applied Optics Beijing Area Major Laboratory Center for Advanced Quantum Studies Beijing Normal University State Key Laboratory of Polymer Materials Engineering College of Polymer Science and Engineering Sichuan University

Understanding the effect of intermolecular interaction on the growth dynamic of active layers is critical for advancing organic solar cells(OSCs). However, the diverse structure of donors and acceptors makes the research challenging. Additives with customizable structures and properties could simplify this complexity. Herein, we meticulously tailor two additives of 3,4-ethylenedioxythiophene(EDOT) and 2,5-dibromo-3,4-ethylenedioxythiophene(DBEDOT), possessing distinct intermolecular interaction features to elaborate the inherent relationship. It is found that varied interaction strengths can alter film formation processes. The enhanced intermolecular interaction between the DBEDOT and non-fullerene acceptor BTP-e C9-4F results in pre-aggregation and longer crystallization duration of BTP-e C9-4F, facilitating the formation of films with compact molecular packing and decent phase separation. Thus, exciton dissociation and charge transport become more efficient. Finally, devices processed with DBEDOT exhibit a remarkable power conversion efficiency of 19.35% in small-area OSCs and 14.11% in bladecoated 5 cm × 5 cm organic solar mini-modules. Especially, OSCs can maintain 80% of their initial efficiency after continuous annealing at 85 °C for over 2,100 h.

关键词： organic solar cell non-fullerene acceptor film growth molecular packing intermolecular interaction

Cyano migration-mediated radical-polar crossover cyclopropanation

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Science China chemistry 2025年第1期68卷 241-248页

作者： Ziqiang Wang Yasu Chen Jie Li Chen Zhu Key Laboratory of Organic Synthesis of Jiangsu Province College of Chemistry Chemical Engineering and Materials ScienceSoochow University Frontiers Science center for Transformative Molecules Zhangjiang Institute for Advanced Study and Shanghai Key Laboratory for Molecular Engineering of Chiral Drugs Shanghai Jiao Tong University

We report a novel cyano migration-mediated radical-polar crossover process, whereby both the sulfonylcyanation of aliphatic alkenes and the formation of cyclopropanes are concurrently achieved. This transformation yields a diverse array of multisubstituted cyclopropanes under mild photocatalytic conditions. Mechanistic studies elucidate that the reaction proceeds via intramolecular nucleophilic substitution, leading to the formation of the cyclopropane derivatives.

关键词： cyclopropanation cyano migration radical-polar crossover radical reactions

Catalyst–Support Interaction in Polyaniline‑Supported Ni_(3)Fe Oxide to Boost Oxygen Evolution Activities for Rechargeable Zn‑Air Batteries

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Nano-Micro Letters 2025年第1期17卷 176-190页

作者： Xiaohong Zou Qian Lu Mingcong Tang Jie Wu Kouer Zhang Wenzhi Li Yunxia Hu Xiaomin Xu Xiao Zhang Zongping Shao Liang An Department of Mechanical Engineering The Hong Kong Polytechnic UniversityHung HomKowloonHong Kong SARPeople’s Republic of China Jiangsu Key Laboratory of atmospheric Environment Monitoring and Pollution Control Jiangsu Collaborative Innovation Center of Atmospheric Environment and Equipment TechnologySchool of Environmental Science and TechnologyNanjing University of Information Science and TechnologyNanjing 210044People’s Republic of China Department of chemistry The Chinese University of Hong KongMa Lin BuildingShatinHong Kong SAR 999077People’s Republic of China WA School of Mines:Minerals Energy and Chemical Engineering(WASM‑MECE)Curtin UniversityPerthWA 6102Australia Research Institute for Advanced Manufacturing The Hong Kong Polytechnic UniversityHung HomKowloonHong Kong SARPeople’s Republic of China Research Institute for Smart Energy The Hong Kong Polytechnic UniversityHung HomKowloonHong Kong SARPeople’s Republic of China

Catalyst–support interaction plays a crucial role in improving the catalytic activity of oxygen evolution reaction(OER).Here we modulate the catalyst–support interaction in polyaniline-supported Ni_(3)Fe oxide(Ni_(3)Fe oxide/PANI)with a robust hetero-interface,which significantly improves oxygen evolution activities with an overpotential of 270 mV at 10 mA cm^(-2)and specific activity of 2.08 mA cm_(ECSA)^(-2)at overpotential of 300 mV,3.84-fold that of Ni_(3)Fe *** is revealed that the catalyst–support interaction between Ni_(3)Fe oxide and PANI support enhances the Ni–O covalency via the interfacial Ni–N bond,thus promoting the charge and mass transfer on Ni_(3)Fe *** the excellent activity and stability,rechargeable Zn-air batteries with optimum Ni_(3)Fe oxide/PANI are assembled,delivering a low charge voltage of 1.95 V to cycle for 400 h at 10 mA cm^(-2).The regulation of the effect of catalyst–support interaction on catalytic activity provides new possibilities for the future design of highly efficient OER catalysts.

关键词： Catalyst-support interaction Supported catalysts Heterointerface Oxygen evolution reaction Zn-air batteries

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Chiral phosphoramidite ligand-modulated palladium auto-tandem catalysis for asymmetric dehydrogenative dienylation of imines with α-alkenes

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Science China chemistry 2025年

作者： Zhong-Sheng Nong Hao-Fan Qian Ying-Chun Chen Pu-Sheng Wang Liu-Zhu Gong Hefei National Research center for Physical Sciences at the Microscale and Department of chemistry University of Science and Technology of China Key Laboratory of Drug Targeting and Drug Delivery System (Sichuan University) Ministry of Education and Sichuan Research Center for Drug Precision Industrial Technology West China School of Pharmacy Sichuan University School of Materials and chemistry Southwest University of Science and Technology

The development of efficient processes allowing rapid access to complex chiral molecules from easily available alkenes is a long-term pursuit in the synthetic chemistry community. Transition metal-catalyzed asymmetric functionalization of allylic C–H bond represents a unique alternative toward this goal. However, enantioselective dehydrogenative transformation of olefins to value-added optically enriched molecules remains yet to be discovered. Here, we report a highly enantioselective dehydrogenative dienylation of imines with unactivated α-alkenes driven by the synergistic action of palladium complex and carboxylic acid. Chiral phosphoramidite ligands turned out to be superior in modulating the performance of palladium autotandem catalysis and allowed a broad range of α-alkenes and imines to be transformed into chiral dienylamines. Mechanistic studies suggest that the dienes could be in situ generated from α-alkenes through a palladium(0)-mediated dehydrogenative process in the presence of excess benzoquinone oxidants, and then participated in the Pd-chiral phosphoramidite-catalyzed intermolecular vinylogous-type addition to the imines activated by the carboxylic acid co-catalyst. Notably, the second β-H elimination occurring in the dienylation event might be the turnover-limiting step.

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高离子电导率和均匀锂离子传输的磺酸基聚醚凝胶聚合物电解质用于高性能锂金属电池（英文）

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Science China Materials 2025年

作者：胡振原刘子莹刘凯秦金鹏郭文凡凡威震张运丰 Hydrogen Energy Technology Innovation center for Hubei Province Faculty of Material Science and Chemistry China University of Geosciences (Wuhan) School of Environmental studies China University of Geosciences (Wuhan)

凝胶聚合物电解质基锂金属电池由于高比容量和低成本的优势,对于发展高能量密度储存设备具有重要意义.然而,传统型凝胶电解质因其锂离子传输效率较低、易产生极化现象,从而导致不可控的锂枝晶生长,最终阻碍了其大规模实际应用.本文设计...

凝胶聚合物电解质基锂金属电池由于高比容量和低成本的优势,对于发展高能量密度储存设备具有重要意义.然而,传统型凝胶电解质因其锂离子传输效率较低、易产生极化现象,从而导致不可控的锂枝晶生长,最终阻碍了其大规模实际应用.本文设计并合成出具有丰富离子传输位点的聚醚型锂单离子传导聚合物（DEBS-Li）,随后将其与聚偏氟乙烯-六氟丙烯P（VDF-HFP）基质相复合,采用静电纺丝技术制备出高传导性复合纳米纤维膜.实验发现,具有丰富磺酸基团的DEBS-Li可通过静电作用促进锂盐解离,从而加快离子迁移,赋予凝胶电解质在25℃时具有高离子电导率(～1.58×10-3S cm-1)和锂离子迁移数（0.62）.离子传输动力学的优化可大大延迟锂枝晶的成核时间,并显著抑制锂枝晶的形成.因此,采用该电解质组装成的锂对称电池在1.5 mA cm-2稳定运行250小时未发生短路,金属锂二次电池在10 C的高倍率下稳定循环500圈,容量保持率约为90%.本工作开发的新型聚醚凝胶聚合物电解质在高性能锂电池的实际应用中具有极大潜力.

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Superhydrophobic and corrosion-resistant siloxane-modified MgAl-LDHs coatings on magnesium alloy prepared under mild conditions

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International Journal of Minerals,Metallurgy and Materials 2025年第2期32卷 450-463页

作者： Wenxi Zhang Zhangzelong Zhuo Dan Xu Liang Wu Zhihui Xie Chemical Synthesis and Pollution Control Key Laboratory of Sichuan Province College of Chemistry and Chemical EngineeringChina West Normal UniversityNanchong 637002China College of Materials Science and Engineering/National Engineering Research center for Magnesium Alloys Chongqing UniversityChongqing 400044China

We have developed a superhydrophobic and corrosion-resistant LDH-W/PFDTMS composite coating on the surface of Mg *** composite comprised a tungstate-intercalated(LDH-W)underlayer that was grown at low temperature(relative to hydrothermal reaction conditions)under atmospheric pressure and an outer polysiloxane layer created from a solution containing perfluorodecyltrimethoxysilane(PFDTMS)using a simple immersion *** successful intercalation of tungstate into the LDH phase and the following formation of the polysiloxane layer were confirmed through X-ray diffraction(XRD),Fourier transform infrared(FTIR)spectroscopy,and X-ray photoelectron spectroscopy(XPS).The corrosion resistance of the LDH-W film,both before and after the PFDTMS modification,was evaluated using electrochemical impedance spectroscopy(EIS),Tafel curves,and immersion *** results showed that Mg coated with LDH-W/PFDTMS exhibited significantly enhanced corrosion protection compared to the unmodified LDHW film,with no apparent signs of corrosion after exposure to 3.5wt%NaCl solution for 15 ***,the LDH-W/PFDTMS coating demonstrated superior superhydrophobicity and self-cleaning properties against water and several common beverages,as confirmed by static contact angle and water-repellency *** results offer valuable insights into preparing superhydrophobic and corrosion-resistant LDH-based composite coatings on Mg alloy surfaces under relatively mild reaction conditions.

关键词： Mg alloy corrosion coating layered double hydroxide

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