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Photoinduced radical sulfur dioxide insertion with asymmetric cyclization of alkenes: accessing β-chiral sulfones bearing S-stereocentric cyclic sulfinamides

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Science China chemistry 2025年第1期68卷 257-263页

作者： Jiapian Huang Chenxin Wang Xu Wang Xiaoyu Zhou Wei Xiao Jie Wu School of Pharmaceutical and Chemical Engineering & institute for Advanced Studies Taizhou University State Key Laboratory of Organometallic chemistry Shanghai Institute of Organic Chemistry Chinese Academy of Sciences School of chemistry and Chemical Engineering Henan Normal University

The generation of various β-chiral sulfones bearing chiral cyclic sulfinamides through photoredox-catalyzed sulfur dioxide insertion with asymmetric radical cyclization is described. This method features a broad substrate scope and excellent stereospecificity. Computational studies reveal that the dispersion interaction between sulfinyl group and CH2SO2Ph group plays a crucial role in the stereoselectivity control.

关键词： β-chiral sulfones chiral cyclic sulfinamides sulfur dioxide insertion asymmetric radical cyclization stereoselectivity

Establishing a new testing protocol of the electrochemical stability window for electric double-layer capacitors

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Science China chemistry 2025年第1期68卷 217-225页

作者： Ruilin Hou Xiaoxi Zhao Tingting Liang Qingyun Dou Shan Xu Xingbin Yan School of Materials Science and Engineering Sun Yat-sen University Laboratory of Clean Energy chemistry and Materials Lanzhou Institute of Chemical Physics Chinese Academy of Sciences College of Engineering and applied Sciences Nanjing University Center of Industrial Analysis and Testing Guangdong Academy of Science

The electrochemical stability window(ESW) is crucial for determining the energy density of electric double-layer capacitors(EDLCs). However, current ESW testing protocols of EDLCs are strongly affected by artificial factors, thereby leading to unreliable result. To solve this problem, we first identify the key shortcomings of the traditional protocols by analyzing their test principles. Subsequently, taking an aqueous carbon-based EDLC as an example, we design a side reaction descriptor to represent the response difference in the charging capacitance to side reactions between the cyclic voltammetry and galvanostatic chargedischarge methods. With the aid of this descriptor, we propose a new ESW testing protocol, which is not only able to completely avoid the adverse influence of subjective factors but also fully consider the operating condition limitations. The protocol can be extended from the single electrode to the full device. This work proposes a more rigorous definition of ESW and provides a reliable protocol for evaluating the ESW of EDLCs.

关键词： electric double-layer capacitors electrochemical stability window testing protocol side reaction descriptor operating limitation

Boosting hydrocarbon conversion via Cu-doping induced oxygen vacancies on CeO2 in CO2 electroreduction

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Journal of Energy chemistry 2025年第1期100卷 66-76页

作者： Lei Xue Tong Shi Chenhui Han Heng Zhang Fenrong Liu Haorun Li Yan Wang Xiaojun Gu Shanghong Zeng Inner Mongolia Key Laboratory of chemistry and Physics of Rare Earth Materials School of Chemistry and Chemical Engineering Inner Mongolia University State Key Laboratory of Coal Conversion Institute of Coal Chemistry Chinese Academy of Sciences institute of Catalysis Department of Chemistry Zhejiang University National Key Laboratory of Baiyunobo Rare Earth Resource Research and Comprehensive Utilization Baotou Research Institute of Rare Earths

Conversion of CO2back to hydrocarbons is the most direct way of closing the“carbon cycle”,and its significance is further enlarged if this process is driven by renewable energies such as ***,precisely controlling the product selectivity towards hydrocarbons against the competitive hydrogen evolution remains challenging,especially for Cu-based ***,we report a novel defect engineering strategy,by which Cu-doping-induced oxygen vacancies on CeO2nanorods were effectively created,with adjustable vacancy/Cu *** resulting optimum catalyst shows up to 79% catalytic current density to hydrocarbons （excluding CO）,with 49% faradaic efficiency to *** and density functional theory unveil that the ratio between oxygen vacancy and Cu affects significantly the formation of*CHO and activation of H2O,which leads to the following deep hydrogenation to *** findings may spur new insights for designing and developing more controllable chemical process relevant to CO2utilization.

关键词： Nanorods

Nitrogen addition promotes soil carbon accumulation globally

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Science China Life Sciences 2025年第1期68卷 284-293页

作者： Xuemei Yang Suhui Ma Erhan Huang Danhua Zhang Guoping Chen Jiangling Zhu Chengjun Ji Biao Zhu Lingli Liu Jingyun Fang institute of Ecology College of Urban and Environmental Sciencesand Key Laboratory for Earth Surface Processes of the Ministry of EducationPeking University Ministry of Education Key Laboratory for Transboundary Ecosecurity of Southwest China School of Ecology and Environmental ScienceYunnan University State Key Laboratory of Vegetation and environmental Change Institute of BotanyChinese Academy of Sciences

Soil is the largest carbon(C) reservoir in terrestrial ecosystems and plays a crucial role in regulating the global C cycle and climate *** nitrogen(N) deposition has been widely considered as a critical factor affecting soil organic carbon(SOC) storage, but its effect on SOC components with different stability remains unclear. Here, we analyzed extensive empirical data from 304 sites worldwide to investigate how SOC and its components respond to N addition. Our analysis showed that N addition led to a significant increase in bulk SOC(6.7%), with greater increases in croplands(10.6%) and forests(6.0%) compared to grasslands(2.1%). Regarding SOC components, N addition promoted the accumulation of plant-derived C(9.7%–28.5%) over microbial-derived C(0.2%), as well as labile(5.7%) over recalcitrant components(–1.2%), resulting in a shift towards increased accumulation of plant-derived labile C. Consistently, N addition led to a greater increase in particulate organic C(11.9%) than mineral-associated organic C(3.6%), suggesting that N addition promotes C accumulation across all pools, with more increase in unstable than stable pools. The responses of SOC and its components were best predicted by the N addition rate and net primary productivity. Overall, our findings suggest that N enrichment could promote the accumulation of plant-derived and non-mineral associated C and a subsequent decrease in the overall stability of soil C pool, which underscores the importance of considering the effects of N enrichment on SOC components for a better understanding of C dynamics in soils.

关键词： meta-analysis nitrogen enrichment soil organic carbon carbon accumulation carbon stability

Simulations of electron zebra stripes in the inner radiation belt using a composite empirical electric field model

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Science China Earth Sciences 2025年第1期68卷 27-38页

作者： Ziyang WANG Ying LIU Qiugang ZONG Hong ZOU Yuguang YE Xuzhi ZHOU Chao YUE Shan WANG institute of Space Physics and applied Technology Peking University State Key Laboratory of Lunar and Planetary Science Macau University of Science and Technology

The phenomenon termed “zebra stripes” manifests as regular patterns in the energy-space(L shell) spectrum of energetic electrons(ranging from tens to hundreds ke V) within the inner radiation belt. These structures exhibit drift-periodic behavior and commonly arise from large-scale electric field perturbations near the substorm onsets. In this study, we introduce a composite electric field model and replicate the formation, structure, and evolution of zebra stripes using a bounce-averaged test particle code under this electric field model. High-resolution measurements of energetic electrons obtained from the Van Allen Probes and the recently launched Macao Science Satellites-1 are used as initial conditions and served to validate our test particle simulations. Comparative analyses between observed data and simulations demonstrate our test particle method's efficacy in capturing zebra stripes' general behavior. Moreover, the composite model proves capable of reproducing realistic variations in the electric field within the inner radiation belt to a certain extent. Nevertheless, subtle differences emerge in the flux strength and the positions of stripes. These disparities primarily stem from limitations inherent in the electric field model and the initial conditions of the simulation. Acknowledging that the model represents an average case, it is conceivable that real-world scenarios may deviate from the average, thereby introducing variations in the observed phenomena.

关键词： Zebra stripes Inner radiation belt Large-scale electric fields Van Allen Probes Macao Science Satellite

Boosting bidirectional sulfur conversion enabled by introducing boron-doped atoms and phosphorus vacancies in Ni2P for lithium-sulfur batteries

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Journal of Energy chemistry 2025年第1期100卷 760-769页

作者： Lin Peng Yu Bai Hang Li Meixiu Qu Zhenhua Wang Kening Sun Advanced Research institute of Multidisciplinary Science Beijing Institute of Technology Beijing Key Laboratory of Chemical Power Source and Green Catalysis School of Chemistry and Chemical Engineering Beijing Institute of Technology

Lithium-sulfur （Li-S） batteries have gained great attention due to the high theoretical energy density and low cost,yet their further commercialization has been obstructed by the notorious shuttle effect and sluggish redox ***,we supply a strategy to optimize the electron structure of Ni2P by concurrently introducing B-doped atoms and P vacancies in Ni2P （Vp-B-Ni2P）,thereby enhancing the bidirectional sulfur *** study indicates that the simultaneous introduction of B-doped atoms and P vacancies in Ni2P causes the redistribution of electron around Ni atoms,bringing about the upward shift of d-band center of Ni atoms and effective d-p orbital hybridization between Ni atoms and sulfur species,thus strengthening the chemical anchoring for lithium polysulfides （LiPSs） as well as expediting the bidirectional conversion kinetics of sulfur ***,theoretical calculations reveal that the incorporation of B-doped atoms and P vacancies in Ni2P selectively promotes Li2S dissolution and nucleation ***,the Li-S batteries with Vp-B-Ni2P-separators present outstanding rate ability of 777 m A h g-1at 5 C and high areal capacity of 8.03 mA h cm-2under E/S of 5μL mg-1and sulfur loading of 7.20 mg *** work elucidates that introducing heteroatom and vacancy in metal phosphide collaboratively regulates the electron structure to accelerate bidirectional sulfur conversion.

关键词： Lithium sulfur batteries

Ni-catalyzed cross-electrophile alkyl-alkyl coupling reactions

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Science China chemistry 2025年

作者： Li-Xu You Lan Tian Chun-Ling Guo Shun-Xi Li Yu-Cheng Liu Yu-Long Li Wei Shu College of chemistry and environmental Engineering Key Laboratory of Green Catalysis of Higher Education Institutes of Sichuan Sichuan University of Science and Engineering Guangming Advanced Research institute Shenzhen Grubbs Institute Department of Chemistry and Guangdong Provincial Key Laboratory of Catalysis Southern University of Science and Technology

Introducing saturated carbon-carbon bonds into organic molecules significantly increases the three-dimensional configuration,thus altering the physical and chemical properties as well as the functions of molecules. Transition-metal-catalyzed carboncarbon cross-couplings represent one of the most straightforward, efficient and modular alternatives to build saturation in a single step. However, the efficient construction of alkyl-alkyl bonds remains a formidable challenge due to the precise manipulation of multiple alkyl metallic intermediates as well as associated competitive side reactions and selectivity control. Over the past years, Ni-catalyzed cross-coupling under reductive conditions has gained more and more attention for alkyl-alkyl crosscoupling partially attributing to the low-valent state of metal centers under reducing conditions, which suppresses the competitive β-hydride elimination process, thus facilitating the formation of alkyl-alkyl bonds. In this review, the initiative and progress of Ni-catalyzed cross-electrophile alkyl-alkyl cross-coupling, including the efforts in racemic and enantioselective formation of alkyl-alkyl bonds, have been summarized and discussed. Moreover, the challenges and further opportunities in this area have also been discussed.

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Late Paleozoic to early Mesozoic volcanic-sedimentary history of the southeastern margin of the Central Asian Orogenic Belt: Timing of uplift of the Inner Mongolia paleo-uplift

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Science China Earth Sciences 2025年第1期68卷 297-309页

作者： Wenxing HAO Jin-Hui YANG Guang ZHU State Key Laboratory of Lithospheric Evolution Institute of Geology and Geophysics Chinese Academy of Sciences School of Resource and environmental Engineering Hefei University of Technology

The Kulun region is located in the eastern Bainaimiao arc belt on the southeastern margin of the Central Asian Orogenic Belt(CAOB), adjacent to the North China Craton(NCC) to the south. This region records the closure of the PaleoAsian Ocean during the Paleozoic to early Mesozoic and is key to study the tectonic evolution of the northern margin of the *** conducted zircon U-Pb geochronology and Hf isotope analysis of volcanic-sedimentary and intrusive rocks in the Kulun region. The volcanic-sedimentary rocks were previously assigned an early Carboniferous age, but include volcanic rocks with ages of 267–266 Ma and sedimentary rocks with youngest detrital zircon age peaks of 265–244 Ma, which were intruded by a granite with an age of 242 Ma. This indicates that these rocks are actually middle Permian to Middle Triassic in age(267–242Ma) and correspond to the Qingfengshan and Liujiagou formations. Moreover, two volcanic rock samples have high εHf(t) values(+1.6 to +16.1) and relatively young two-stage Hf model ages(1095–327 Ma), indicating their sources associated with the CAOB. The age spectra and Hf isotopic characteristics of detrital zircons from the sedimentary rocks suggest that, during the middle Permian to Middle Triassic, the sedimentary provenance in the Kulun region was mainly the CAOB. However, by the Early Jurassic, the provenance changed to the NCC(i.e., the Inner Mongolia Paleo-uplift, IMPU). This result, combined with the development of a series of conglomerates on the northern margin of the NCC in the Late Triassic(i.e., Xingshikou, Xiaoyingzi,and Xiaohekou formations), indicates the Kulun region experienced an abrupt change in paleogeography during the Late Triassic, with the IMPU undergoing significant uplift and thus becoming the main sediment source in the Kulun region. Based on the Late Triassic alkaline igneous belt(235–215 Ma) in the IMPU, we speculate that this uplift was caused by detachment of the southward-subducting Paleo-Asian oceanic

关键词： Central Asian Orogenic Belt the North China Craton Zircon geochronology Hf isotopes Inner Mongolia Paleo-uplift

Recent progress on photoactive nonprecious transition-metal complexes

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Science China chemistry 2025年第1期68卷 46-95页

作者： Zhong-Liang Gong Hong-Jie Zhang Yan Cheng Jianxun Liu Yuhan Ai Yaqin Li Zhihui Feng Qiong Zhang Shaolong Gong Yong Chen Chang-Jiang Yao Yuan-Yuan Zhu Liang-Jin Xu Yu-Wu Zhong CAS Key Laboratory of Photochemistry Institute of Chemistry Chinese Academy of Sciences State Key Laboratory of Structural Cemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences School of chemistry and Chemical Engineering Anhui Key Laboratory of Advanced Catalytic Materials and Reaction EngineeringHefei University of Technology State Key Laboratory of Explosion Science and Safety Protection School of Mechatronical Engineering Beijing Institute of Technology College of chemistry and Molecular Sciences Hubei Key Lab on Organic and Polymeric Optoelectronic Materials Wuhan University School of chemistry and Chemical Engineering Anhui University Key Laboratory of Photochemical Conversion and Optoelectronic Materials & CAS-HKU Joint Laboratory on New Materials Technical Institute of Physics and Chemistry Chinese Academy of Sciences

Photoactive complexes of nonprecious transition metals, mainly including those in the first-row and partially the second-row of the Periodic table of elements, have received increasing attention in view of their low cost and long-term sustainability. They are recognized as promising alternatives to noble transition metal complex congeners that have been extensively studied in optoelectronic devices, artificial photosynthesis, photocatalysis, biodiagnostics, and therapeutics, etc. This review is devoted to a comprehensive summary on the classical and recent advances on photoactive nonprecious transition metal complexes, including photoactive Zr, V, Cr, Mo, and W complexes, Mn complexes and hybrids, Fe, Co, Ni, and Cu complexes, and Zn and Cd complexes and hybrids. A particular focus is given on the molecular design, modulation of photophysical and photochemical properties, and applications of the representative and lately-developed nonprecious metal complexes. In addition, a perspective on the future development in this field is provided at the end of this review.

关键词： photoactive metal complexes earth-abundant metals nonprecious metal complexes luminescence photochemistry