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Visible-light-responsive homologous heterostructure of oxynitrides constructed to boost charge separation and water splitting

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Science China chemistry 2025年第1期68卷 186-191页

作者： Hai Zou Yunfeng Bao Xueshang Xin Yu Qi Tengfeng Xie Fuxiang Zhang State Key Laboratory of Catalysis Dalian National Laboratory for Clean Energy Dalian Institute of Chemical Physics Chinese Academy of Sciences school of chemistry and chemical engineering Liaoning Normal University college of chemistry Jilin University

Constructing type II heterostructures represents a widely recognized strategy for enhancing charge separation and photocatalytic efficiency,but it remains challenging to fabricate homologous heterostructures based on visible-light-responsive semiconductors,especially for popularly investigated （oxy）nitrides with low thermal ***,we synthesized a homologous heterostructure （denoted as YTON＿H） based on the oxynitrides of YTaO4-xNyand YTa *** heterostructure exhibits type II band structure alignment and intimate interface achieved through a magnesium （Mg） powder-assisted nitridation *** with widely reported heterologous heterostructures,the as-obtained YTON＿H homologous heterostructure could similarly exhibit enhanced charge separation as well as photocatalytic water splitting performance with respect to its counterparts(YTaO4-xNyand YTaON2).Meanwhile,detailed structural characterizations and spectroscopy analysis have been made to confirm the formation of heterostructure and promotion of spatial charge separation.

关键词： charge separation heterostructure oxynitride photocatalysis visible light

Discovery of a new family member of arsenic–vanadium polyoxometalates with high catalytic performance for one-pot coupling of CO2, epoxides and amines

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Tungsten 2025年第1期7卷 80-87页

作者： Fang-Qian Wang Yin Zhang Wei-Wei Wang Mei-Qian Fu Hong-Bing Mo Wei-Dong Yu Chao Liu Jun Yan college of chemistry and chemical engineering Central South University Junior Education Department Changsha Normal University school of Science Hunan University of Technology and Business

Arsenic-vanadium polyoxometalates（POMs） represent a family of tremendous potential catalysts owing to their peculiar physical and chemical *** in CO2conversion,using POMs to catalyze the conversion of CO2and epoxide into chemical intermediates is the research ***,A new family number of arsenic-vanadium POMs,[N（CH3）4]4[As8V12O38（H2O）]·2H2O({As8V12O38}),was reported and characterized by single-crystal X-ray diffraction,fourier transform infrared spectroscopy,X-ray photoelectron spectroscopy,*** from other allotropicity,{As8V12O38}shows a different structure pattern with an I-43d *** obtained {As8V12O38} was employed as a catalyst for the *** initial catalytic reaction confirmed that {As8V12O38} can catalyze the formation of epoxy carbonate by using 1.01 kPa CO2and epoxide at 70℃.Furtherly,when added amine in the catalytic system,oxazolidinone could be obtained by high yields,which provides an efficient way to convert CO2into profitable ***,a possible catalytic reaction mechanism was proposed by using different characterization analyses.{As8V12O38} first catalyzes the epoxide and CO2to form an epoxy carbonate and then catalyzes epoxy carbonate and benzylamine into oxazolidinone.

关键词： Arsenic CO2 conversion Oxazolidinone Polyoxometalates Vanadium

Facile synthesis of the dodecahydridododecaborate (B12H122-) from borane Lewis base adducts

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Science China chemistry 2025年

作者： Yi Jing Xin-Ran Liu Xing-Hua Wang Hui Han Sha-Sha Liang Xi-Meng Chen Dong-Hui Wei Lai-Sheng Wang Xue-Nian Chen college of chemistry Zhengzhou University school of chemistry and chemical engineering Henan Key Laboratory of Boron Chemistry and Advanced MaterialsHenan Normal University Department of chemistry Brown University

Polyhedral boranes are a class of well-known boron molecular clusters widely used in energy,chemistry,medicine,and materials science because of their unique physical and chemical *** efforts have been made in the past decades to find more effective synthetic methods for this important class of boron ***,existing synthetic methods suffer from low efficiency and low ***,we report a facile one-pot synthesis of[（CH3）3S]2B12H12with moderate yields at mild *** mechanisms for the multi-step chemoselective synthesis of B12H122-without other by-products are elucidated based on theoretical results and our previous *** Lewis base used in B–H bond condensation reaction,which acts as a hydrogen or to balance the newly generated polyhedral borane charges,is proposed and studied in *** current study has led to a more effective and selective synthetic method for B12H122-and has also implicated the syntheses of other new polyhedral boranes.

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Identifying the dynamic behaviors in complete reconstruction of Co-based complex precatalysts during electrocatalytic oxygen evolution

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Journal of Energy chemistry 2025年第1期100卷 226-233页

作者： Jingfang Zhang Danyang Wu Linke Cai Youluan Lu Fanpeng Cheng Lijuan Shi Qun Yi Yao Liu Yi Huang Key Laboratory of Green chemical engineering Process of Ministry of Education Engineering Research Center of Phosphorus Resources Development and Utilization of Ministry of Education Hubei Key Laboratory of Novel Reactor and Green Chemical Technology School of Chemical Engineering & Pharmacy Wuhan Institute of Technology Key Laboratory of Pesticide & chemical Biology of Ministry of Education Engineering Research Center of Photoenergy Utilization for Pollution Control and Carbon Reduction of Ministry of Education College of Chemistry Central China Normal University college of Materials Science and engineering Fuzhou University

Transition metal-based nanomaterials have emerged as promising electrocatalysts for oxygen evolution reaction（OER）. Considerable research efforts have shown that self-reconstruction occurs on these nanomaterials under operating conditions of OER process. However, most of them undergo incomplete reconstruction with limited thickness of reconstruction layer, leading to low component utilization and arduous exploration of real catalytic mechanism. Herein, we identify the dynamic behaviors in complete reconstruction of Co-based complexes during OER. The hollow phytic acid（PA） cross-linked CoFe-based complex nanoboxes with porous nanowalls are designed because of their good electrolyte penetration and mass transport ability, in favor of the fast and complete reconstruction. A series of experiment characterizations demonstrate that the reconstruction process includes the fast substitution of PA by OH-to form Co（Fe）(OH)xand subsequent potential-driven oxidation to Co（Fe）OOH. The obtained CoFeOOH delivers a low overpotential of 290 mV at a current density of 10 mA cm-2and a long-term *** experiment results together with theory calculations reveal that the Fe incorporation can result in the electron rearrangement of reconstructed CoFeOOH and optimization of their electronic structure,accounting for the enhanced OER activity. The work provides new insights into complete reconstruction of metal-based complexes during OER and offers guidelines for rational design of high-performance electrocatalysts.

关键词： Oxygen evolution reaction

Bifunctional bridging capping layer enables 24.5% efficiency of perovskite solar cells with polymer-based hole transport materials

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Science China chemistry 2025年第1期68卷 350-359页

作者： Can Zhu Yiyang Wang Lei Meng Beibei Qiu Jing Li Shucheng Qin Ke Hu Xin Jiang Wenbin Lai Minchao Liu Zhe Liu Chenxing Lu Jinyuan Zhang Yongfang Li Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Organic Solids Institute of Chemistry Chinese Academy of Sciences school of chemical Science University of Chinese Academy of Sciences Key Laboratory of Solid State Optoelectronic Devices of Zhejiang Province College of Physics and Electronic Information Engineering Zhejiang Normal University Key Laboratory of Photochemical Conversion and Optoelectronic Materials Technical Institute of Physics and ChemistryChinese Academy of Sciences Laboratory of Advanced Optoelectronic Materials College of Chemistry Chemical Engineering and Materials ScienceSoochow University

Developing a bridge capping layer between perovskite and hole transport layer materials（HTMs） in the n-i-p perovskite solar cells（pero-SCs） is an effective approach to modify the morphology of HTMs and passivate the perovskite ***, we select the quinoxaline-based bifunctional passivation agent, quinoxalin-6-yl-methylamine hydrochloride（Qx MACl）,as the bridging layer, and a D-A copolymer PBQ12 containing the same quinoxaline unit as an HTM for the n-i-p pero-SCs. Due to the π-π stacking among the common quinoxaline units in the bridge layer and HTM, Qx MACl induces the π-π stacking of the PBQ12 film and improves the film morphology of HTMs with better conductivity. Additionally, Qx MACl can effectively passivate the perovskite surface, and PBQ12 possesses appropriate energy levels and high hole mobility. The pero-SCs based on FAPbI3with PBQ12/Qx MACl treatment showed a higher power conversion efficiency（PCE） of 24.05% and outstanding stability, maintaining 95.4% and 92.1% of its initial PCE after 750 h of storage and after over 800 h of thermal annealing at 85 °C, respectively. To further enhance the PCE of the PBQ12/Qx MACl-based devices, we developed a non-metal ion dopant for the PBQ12 HTM. Through trace doping of PBQ12 HTM by the non-metal ion dopant, the PCE of the PBQ12/Qx MACl-based devices reached 25.24%（the calibrated PCE of 24.55% by the National Institute of Metrology, China）.

关键词： D-A copolymer, hole transport materials, bifunctional bridge capping layer, passivation perovskite solar cells

Asymmetric interfacial engineering regulated charge distribution on Ru/Ni-N-C sites for efficient hydrogen evolution reaction in alkaline and seawater electrolytes

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Science China chemistry 2025年

作者： Rui Yu Xi Cao Chengyang Zhu Qingqing Chen Ziyi Yan Binbin Jiang Junjie Mao Xianwen Wei Key Laboratory of Electrochemical Clean Energy of Anhui Higher Education Institutes College of Chemistry and Materials ScienceAnhui Normal University Anhui Provincial Key Laboratory of Advanced Catalysis and Energy Materials School of Chemistry and Chemical Engineering Anqing Normal University school of chemistry and chemical engineering Anhui University of Technology

Developing highly efficient and cost-effective electrocatalysts for hydrogen evolution reaction（HER） is grandly challenging in alkaline and alkaline seawater electrolytes. Herein, the asymmetric interfacial active sites with Ru nanoparticles and Ni single atoms in Ru/Ni-N-C were designed through a solvothermal-pyrolysis process. Constructing highly asymmetric interfacial active sites with a strong electron delocalization effect significantly improves HER kinetics. As expected, Ru/Ni-N-C requires low overpotentials with around 20 mV at 10 mA cm-2and robust durability over 48 h in alkaline and alkaline seawater *** at 200 mA cm-2, the overpotentials are close to 100 mV in both above electrolytes for Ru/Ni-N-C. Density function theory calculation results suggest that the asymmetric interface between Ru nanoparticle and Ni-N-C could accelerate the dissociation of water molecules and modulate the hydrogen species, consequently improving the HER performances. This work opens a unique approach for constructing advanced materials for energy conversion.

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Metastable seed-crystals: epitaxial growth of branched-array organic heterostructure nanowires

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Science China chemistry 2025年

作者： Jin Feng Zhen-Yu Geng Ting-Yao Song Ying-Xin Ma Chuan-Zeng Wang Wei Zhang Hong-Tao Lin Jin Zhou Shu-Ping Zhuo Shu-Hai Chen Xue-Dong Wang school of chemistry and chemical engineering Shandong University of Technology Institute of Functional Nano & Soft Materials (FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials & DevicesSoochow University college of chemistry and chemical engineering Hunan Normal University

Tunable light–matter interactions are exhibited by organic low-dimensional crystals, making these crystals a promising platform for organic photonics. However, the precise synthesis of organic low-dimensional crystals remains challenging due to the stochastic nature of molecular nucleation processes. Herein, the directed nucleation process is driven by the introduction of metastable seed-crystals as the trunk, which ultimately leads to branched-array organic heterostructures. The successful formation of organic heterostructures with high-density branched arrays is attributed to the highest attachment energy (Eatt（023）=-104.25 kcal mol-1) of the exposed （023） crystal plane during the seed-crystal growth route. Significantly, these as-prepared heterostructures inherently have an ultralow lattice mismatch ratio η of 0.7%between trunk and branch, which contributes to the multi-channel photon transportation. Therefore, this work provides valuable insights into a versatile synthetic strategy for accessing low-dimensional heterostructures for integrated optoelectronics.

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Tailor-made high elasticity and low-hysteresis hydrogels based on asymmetric H-bonding crosslinking for wearable applications

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Science China chemistry 2025年

作者： Xiaofang Shi Nan Shi Miaomiao Dang Chengyu Ji Yingjie Li Peiyi Wu Zhiguo Hu Collaborative Innovation Centre of Henan Province for Green Manufacturing of Fine chemicals Henan Engineering Laboratory of Chemical Pharmaceutical and Biomedical Materials School of Chemistry and Chemical Engineering Henan Normal University State Key Laboratory for Modification of chemical Fibers and Polymer Materials College of Chemistry Chemical Engineering and Biotechnology & Center for Advanced Low-dimension Materials Donghua University

The conventional method of fabricating hydrogels constantly confronts the conflict between elasticity and toughness, limiting their repetitive application. Achieving the desired elasticity through a simple and low-cost approach is a significant challenge for hydrogels, particularly through rational molecular design. Here, low-hysteresis and high-toughness hydrogels are developed from the design of a new feature monomer, N-acryloylethylsemicarbazide (NACE). Based on a concept of “asymmetric Hbonding design”, the unique double and triple H-bonding of NACE can result in a novel asymmetric crosslinking polymer with alternating strong and weak H-bonding regions. The NACE is copolymerized with acrylamide (AM) to regulate the mechanical properties of hydrogel via H-bonding density. The P(NACE-AM) ionic hydrogels are obtained simply and rapidly via one-step photopolymerization without a chemical cross-linking agent. The P(NACE-AM) hydrogels combine superb mechanical elasticity and toughness, and excellent ionic conductivity, showing great potential as durable ionic conductive devices for wearable utilization.

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Encapsulating perovskite quantum dots into 3D COF for visible light-driven CO2 reduction

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Science China chemistry 2025年

作者： Xinxin Wang Yucheng Jin Xiya Yang Qingyu Luan Tianyu Wang Dongdong Qi Kang Wang Jianzhuang Jiang college of chemistry and Materials Science Anhui Normal University Beijing Advanced Innovation Center for Materials Genome engineering Beijing Key Laboratory for Science and Application of Functional Molecular and Crystalline Materials Department of Chemistry and Chemical Engineering School of Chemistry and Biological EngineeringUniversity of Science and Technology Beijing

Lead halide perovskite quantum dots（LHP QDs） have been revealed to possess great potential in photocatalytic applications including CO2reduction, which however suffer from poor stability. Herein, a high crystalline hydrazine-linked three-dimensional（3D） covalent organic framework, USTB-17, was fabricated from the reaction between 12-connected building block and 4-connected 3,5,7-tetrakis（4-aldophenyl）-adamantane. Post-modification with Ni2+affords the metallic framework USTB-17（Ni）followed by sequential deposition of the CH3NH2PbI3（MAPbI3） perovskite QDs into its pores, generating the USTB-17（Ni）@MAPbI3composite. Powder X-ray diffraction analysis together with theoretical simulations and transmission electron microscopy discloses the crystalline nature of USTB-17, USTB-17（Ni）, and USTB-17（Ni）@MAPbI3with an unprecedented noninterpenetrated hpt topology. The close contact of QDs inside the COF pores with the Ni catalytic site locating at the pore surface of COF allows a rapid transfer of the photogenerated electrons in QDs to the Ni catalytic sites, enhancing the photocatalytic activity for CO2reduction. This endows USTB-17（Ni）@MAPbI3with efficient photocatalysis performance for photocatalytic CO2reduction with CO generation rate of 365 μmol g-1h-1and CO selectivity up to 96% under visible-light irradiation, 7 times higher than that of USTB-17（Ni）. After four cycles of reactions, the photocatalytic CO generation rate remains almost unchanged, demonstrating its excellent cycle stability.

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