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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

Crustal magma oxidation state and endowments in porphyry copper deposits

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Science China Earth sciences 2025年第1期68卷 226-236页

作者： Yumin AI Massimo CHIARADIA Chao WU Huayong CHEN Key Laboratory of Mineralogy and Metallogeny Guangzhou Institute of Geochemistry Chinese Academy of Sciences University of Chinese Academy of sciences department of Earth sciences University of Geneva Guangdong Provincial Key Laboratory of Mineral Physics and materials

Porphyry copper deposits（PCDs） supply the majority of the world's copper（Cu） as well as significant amounts of molybdenum（Mo） and gold（Au）. The formation of these deposits is controlled by a variety of geological factors, among which the magmatic oxidation is one of the focuses of current research. This study investigates the redox characteristics of arc magmas by analyzing the ratio of vanadium（V） to scandium（Sc） and its correlation with the oxygen fugacity （fO2） of magmas from arcs of various crustal thicknesses globally. We compiled an extensive dataset of published V/Sc values and studied the partition coefficients of Vand Sc between minerals and silicate melts across various magmatic environments. The results demonstrate that fractional crystallization of magnetite markedly reduces V/Sc values of the residual melt. Furthermore, magnesium number（Mg#） at the onset of magnetite fractionation is strongly positively correlated with fO2of the equilibrium magma. Based on this,the oxidation of arc magmas from different crustal thicknesses can be evaluated. The result suggests that magmas generated in crusts thicker than 20 km tend to be more oxidized with increasing crust thickness. This trend is attributed to enhanced intracrustal differentiation processes involving garnet and amphibole, particularly in mature island and continental arcs. In contrast,magmas in thinner arc crusts（materials, display higher oxidation states than most of their thicker crust counterparts. These findings suggest that both subduction dynamics and crustal thickness play a vital role in determining the oxidation state of arc magmas and, consequently, their capacity to generate PCDs. Highly oxidized, primitive arc magmas are less favorable for PCD formation due to that they tend to experience magnetite fractionation and thus sulfide saturation in the early stage of magma evolution, a process leading to copper depletion. On the contra

关键词： Magma evolution V/Sc systematics Magnetite Oxygen fugacity Porphyry copper deposits

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

Boosting Oxygen Evolution Reaction Performance on NiFe‑Based Catalysts Through d‑Orbital Hybridization

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Nano-Micro Letters 2025年第1期17卷 281-292页

作者： Xing Wang Wei Pi Sheng Hu Haifeng Bao Na Yao Wei Luo State Key Laboratory of New Textile materials and Advanced Processing Technology Key Laboratory of New Textile Materials and Applications of Hubei ProvinceSchool of Materials Science and EngineeringWuhan Textile UniversityWuhan 430200People’s Republic of China College of Chemistry and molecular sciences Wuhan UniversityWuhan 430072People’s Republic of China

Anion-exchange membrane water electrolyzers(AEMWEs)for green hydrogen production have received intensive attention due to their feasibility of using earth-abundant NiFe-based *** introducing a third metal into NiFe-based catalysts to construct asymmetrical M-NiFe units,the d-orbital and electronic structures can be adjusted,which is an important strategy to achieve sufficient oxygen evolution reaction(OER)performance in ***,the ternary NiFeM(M:La,Mo)catalysts featured with distinct M-NiFe units and varying d-orbitals are reported in this *** and theoretical calculation results reveal that the doping of La leads to optimized hybridization between d orbital in NiFeM and 2p in oxygen,resulting in enhanced adsorption strength of oxygen intermediates,and reduced rate-determining step energy barrier,which is responsible for the enhanced OER *** critically,the obtained NiFeLa catalyst only requires 1.58 V to reach 1 A cm^(−2) in an anion exchange membrane electrolyzer and demonstrates excellent long-term stability of up to 600 h.

关键词： NiFe-based catalysts d-orbital coupling Oxygen evolution reaction Anion exchange membrane electrolyzer

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Mainchain conformation ordering self-assembly tailored room temperature phosphorescence emission

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Science China Chemistry 2025年第1期68卷 329-336页

作者： Yuzhu Li Yumeng Gao Feng Tian Yu Wang Yuan Yao Shaoliang Lin Xiang Ma Binbin Xu Shanghai Key Laboratory of Advanced Polymeric materials Key Laboratory for Ultrafine Materials of Ministry of Education School of Materials Science and Engineering East China University of Science and Technology Shanghai Synchrotron Radiation Facility Shanghai Advanced Research Institute Chinese Academy of Sciences Key Laboratory for Advance materials and Feringa Noble Prize Scientist Joint Research Centre Frontiers Science for Materiobiology and Dynamic Chemistry School of Chemistry and Molecular Engineering East China University of Science & Technology

Developing organic room-temperature phosphorescence （RTP） materials with a wide range of tunable-emission is significant in expanding the applications of RTP ***,we rationally designed amphiphilic alternating copolymers poly(1,2-bis（4-alkoxyphenyl）ethane-1,2-dione-alt-（ethylene glycol）x)(P（Bz-alt-EGx）) that combined the advantage of alternating benzil and EGxskeleton,and tunable mainchain *** a mainchain conformation ordering assembly （COA） process,P（Bz-alt-EGx） self-assembled into well-defined platelets,and such assemblies emitted blue RTP at ca.425 nm due to the ordered folded-chain conformation and confined *** contrast,traditional self-assembly （TA） of P（Bz-alt-EGx） obtained less ordered aggregates,such as asymmetric worms,vesicles,and rod-like *** resultant less ordered aggregates exhibited yellow-green RTP at ca.550 *** wide-tuning RTP emission in solution （between blue and yellow-green,over125 nm） is realized using the P（Bz-alt-EGx） alternating copolymers under the treatment of different self-assembly *** study uncovers a new strategy to tailor the RTP emission through different self-assembly pathways and holds great promise for the fabrication of advanced optical materials.

关键词： self-assembly conformation ordering alternating copolymer phosphorescence emission

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

Investigations of liquid-liquid transitions in metallic melts by fast differential scanning calorimetry

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Science China(Physics,Mechanics & Astronomy) 2025年

作者： Qi Cheng Yonghao Sun Weihua Wang Beijing National Laboratory for molecular sciences College of Chemistry and Molecular Engineering Peking University School of Physics and Electronic Information Anhui Normal University Institute of Physics Chinese Academy of Sciences Songshan Lake materials Lab

Liquid-liquid transition in metallic melts is an intriguing phenomenon often confused with liquid-liquid separation, oxidation or precipitation. Here, we employ a state-of-the-art ultrafast chip-based differential scanning calorimeter to investigate the thermal behavior of six metallic melts, ranging from unary to quinary systems, at temperatures above their liquidus. Calorimetric signals of liquid-liquid transition vary across systems: Sn melts showed no direct endothermic or exothermic events, though liquid-liquid transition influenced solidification and melting temperatures, while Yb-Zn melts exhibited an exothermic peak during cooling,indicating liquid-liquid transition. Thermal signals in other systems including Li, Pd-Ni-P, Yb-Mg-Zn-Cu and Au-Ag-Pd-Cu-Si,are primarily driven by compositional changes. Our in-situ analysis provides new insights into the structural and compositional evolution of metallic melts, offering significant implications for the design and processing of novel materials.

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Magnetron sputtered nickel oxide with suppressed interfacial defect states for efficient inverted perovskite solar cells

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Journal of Energy Chemistry 2025年第1期100卷 348-355页

作者： Guoqiang Ma Qin Tan Zhaoning Li Jingwei Xiu Jiafeng Wang Tianle Cheng Dong He Qiang Sun Xuhang Ma Francesco Lamberti Zhubing He department of materials Science and Engineering Institute of Innovative Materials (I2M) Shenzhen Key Laboratory of Full Spectral Solar Electricity Generation (FSSEG)Southern University of Science and Technology (SUSTech) Core Research Facilities Southern University of Science and Technology department of Chemical sciences Department of Industrial Engineering University of Padova

Widely used spin-coated nickle oxide （NiOx） based perovskite solar cells often suffer from severe interfacial reactions between the NiOxand adjacent perovskite layers due to surface defect states,which inherently impair device performance in a long-term view,even with surface molecule *** this study,we developed high-quality magnetron-sputtered NiOxthin films through detailed process optimization,and compared systematically sputtered and spin-coated NiOxthin film surfaces from materials to *** sputtered NiOxfilms exhibit improved crystallinity,smoother surfaces,and significantly reduced Ni3+or Ni vacancies compared to their spin-coated ***,the interface between the perovskite and sputtered NiOxfilm shows a substantially reduced density of defect *** solar cells （PSCs） fabricated with our optimally sputtered NiOxfilms achieved a high power conversion efficiency （PCE） of up to 19.93%and demonstrated enhanced stability,maintaining 86.2% efficiency during 500 h of maximum power point tracking under one standard sun ***,with the surface modification using (4-(2,7-dibromo-9,9-dimethylacridin-10（9H）-yl)butyl)p hosphonic acid （DMAcPA）,the device PCE was further promoted to 23.07%,which is the highest value reported for sputtered NiOxbased PSCs so far.

关键词： Perovskite

Ca2+ cation-mediated microenvironment for electrochemical hydrodimerization of furfural

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Science China Chemistry 2025年

作者： Wei Du Shuangshuang Cha Can Lei Mengxin Qu Zhongqiang Deng Ming Gong Xinhe Bao department of Chemistry and Shanghai Key Laboratory of molecular Catalysis and Innovative materials Fudan University State Key Laboratory of Catalysis National Laboratory for Clean Energy Collaborative Innovation Center of Chemistry for Energy Materials Dalian Institute of Chemical Physics Chinese Academy of Sciences

Furfural is one of the most important biomass-based platform molecules as sustainable precursors for chemicals and fuels. The electrochemical hydrodimerization of furfural can generate hydrofuroin, which is a promising precursor for gasoline or jet ***, steering the selectivity toward hydrodimerization under near-neutral conditions that suppress polymerization and disproportionation of furfural remains challenging. Herein, we discovered that tuning the electrolyte cations could be an effective and alternative strategy for modulating furfural reduction to the traditional electrocatalyst design. Under the optimal Ca2+cations,hydrofuroin yield could be much improved from other cations with hydrofuroin selectivity of 95.5%. The systematic characterization of the ion-centered double layer reflected the suitable sizes and charges of hydrated Ca2+for suppressing the hydrogen evolution reaction from activation of surrounding water molecules as well as encouraging furfural accumulation via non-covalent interaction for directing the electron transfer to furfurals. Ions with smaller or larger sizes can either activate local water molecules or form a crowded ionic interface that casts an adverse effect on furfural enrichment. This work not only presents an effective strategy for facilitating biomass valorization via hydrodimerization but also emphasizes the essential role of the ion-centered microenvironment for steering the electrocatalytic pathways.

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