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Crystallization Thermodynamics Regulation of 1.85 eV Wide-Bandgap Perovskite for Efficient and Stable Perovskite-Organic Tandem Photovoltaics

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Angewandte Chemie 2025年

作者： Guanshui Xie Dr. Huan Li Jun Fang Xin Wang Haichen Peng Dr. Dongxu Lin Nuanshan Huang Lin Gan Prof. Wenjia Li Ruixuan Jiang Prof. Tongle Bu Prof. Fuzhi Huang Prof. Sisi He Prof. Longbin Qiu Department of Mechanical and Energy Engineering SUSTech Energy Institute for Carbon Neutrality Southern University of Science and Technology Shenzhen 518055 China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 P. R. China Shenzhen Key Laboratory of Flexible Printed Electronics Technology School of Science Harbin Institute of Technology (Shenzhen) University Town Shenzhen Guangdong 518055 China

Wide-band gap perovskite with adjustable band gaps can be integrated with organic solar cells to form tandem solar cells (TSCs), thereby surpassing the Shockley–Queisser limit. However, increasing Br content to elevate the band gap above 1.8 eV complicates crystallization, leading to inferior film quality and defects due to the unmanageable evolution of intermediate phases. Surface passivation improves crystallization but hard to moderate the inhomogeneous component distributions and defects in the bulk phase. Here, we introduce a diammonium salt as an additive to regulate the homogeneity and crystallization of perovskite film, eliminating the low-dimensional intermediate phase for orientated crystallization of 1.85 eV perovskite, resulting in efficient wide-band gap perovskite solar cells with an impressive open-circuit voltage ( V oc ) of 1.379 V and operational stability remaining 85 % of their initial efficiency after illumination for 1200 h. Furthermore, perovskite-organic TSCs achieve a champion power conversion efficiency of 24.03 % and a high V oc of 2.108 V, one of the highest V oc for perovskite-organic TSCs.

关键词： Wide-band gap perovskite Low-dimensional intermediate phase Suppressed phase segregation Reduced voltage loss Perovskite-organic tandem solar cells

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Symmetry-Broken Ru Nanoparticles with Parasitic Ru-Co Dual-Single Atoms Overcome the Volmer Step of Alkaline Hydrogen Oxidation

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Angewandte Chemie 2024年第12期136卷

作者： Xueqin Q. Mu Prof. Suli L. Liu Mengyang Y. Zhang Zechao C. Zhuang Ding Chen Yuru R. Liao Hongyu Y. Zhao Prof. Shichun C. Mu Dingsheng S. Wang Prof. Zhihui H. Dai School of Chemistry and Molecular Engineering Nanjing Tech University Nanjing 211816 P. R. China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 P. R. China Engineering Research Center of Advanced Rare Earth Materials Department of Chemistry Tsinghua University Beijing 100084 P. R. China

Efficient dual-single-atom catalysts are crucial for enhancing atomic efficiency and promoting the commercialization of fuel cells, but addressing the sluggish kinetics of hydrogen oxidation reaction (HOR) in alkaline media and the facile dual-single-atom site generation remains formidable challenges. Here, we break the local symmetry of ultra-small ruthenium (Ru) nanoparticles by embedding cobalt (Co) single atoms, which results in the release of Ru single atoms from Ru nanoparticles on reduced graphene oxide (Co 1 Ru 1,n /rGO). In situ operando spectroscopy and theoretical calculations reveal that the oxygen-affine Co atom disrupts the symmetry of ultra-small Ru nanoparticles, resulting in parasitic Ru and Co dual-single-atom within Ru nanoparticles. The interaction between Ru single atoms and nanoparticles forms effective active centers. The parasitism of Co atoms modulates the adsorption of OH intermediates on Ru active sites, accelerating HOR kinetics through faster formation of *H 2 O. As anticipated, Co 1 Ru 1,n /rGO exhibits ultrahigh mass activity (7.68 A mg Ru −1 ) at 50 mV and exchange current density (0.68 mA cm −2 ), which are 6 and 7 times higher than those of Ru/rGO, respectively. Notably, it also displays exceptional durability surpassing that of commercial Pt catalysts. This investigation provides valuable insights into hybrid multi-single-atom and metal nanoparticle catalysis.

关键词： dual-single-atom catalysts hydrogen oxidation reaction symmetry-breaking parasitic Ru nanoparticles

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Activation of subnanometric Pt on Cu-modified CeO2 via redox-coupled atomic layer deposition for CO oxidation (vol 11, 4240, 2020)

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NATURE COMMUNICATIONS 2020年第1期11卷 1-8页

作者： Liu, Xiao Jia, Shuangfeng Yang, Ming Tang, Yuanting Wen, Yanwei Chu, Shengqi Wang, Jianbo Shan, Bin Chen, Rong State Key Laboratory of Digital Manufacturing Equipment and Technology School of Mechanical Science and Engineering Huazhong University of Science and Technology Wuhan People’s Republic of China State Key Laboratory of Materials Processing and Die and Mould Technology School of Materials Science and Engineering Huazhong University of Science and Technology Wuhan People’s Republic of China School of Physics and Technology Center for Electron Microscopy MOE Key Laboratory of Artificial Micro- and Nano-structures and Institute for Advanced Studies Wuhan University Wuhan People’s Republic of China General Motors Global Research and Development Chemical Sciences and Materials Systems Lab Warren USA Department of Chemical and Biomolecular Engineering Clemson University Clemson USA Institute of High Energy Physics Chinese Academy of Sciences Beijing People’s Republic of China

A Correction to this paper has been published: 10.1038/s41467-020-19663-3.

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TiO 2 nanofluid infused nanocoating for long-term anti-corrosion

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Chemical Physics Letters 2023年 830卷

作者： Zi-Yan Xu Jing-jing Xie Hao Yu Yang Ge Wei Geng Xiao-Yu Yang State Key Laboratory of Advanced Technology for Materials Synthesis and Processing & Shenzhen Research Institute & Laoshan Laboratory Wuhan University of Technology Wuhan 430070 PR China School of Chemical Engineering and Technology Sun Yat-Sen University 2 Daxue Road Zhuhai 519082 PR China

Marine corrosion has been a global problem with the damage on environment, and economy. With the development, traditional coating technology is difficult to meet the current demands of applications. In this study, TiO 2 nanoparticles were modified and dispersed in silicone oil to form TiO 2 nanofluid. And, the nanofluid was infused into hierarchical structure to produce the SLIPS which is obtained by spraying with the solution of Al 2 O 3 , which significantly reduce the lubricant leaching. As synthesized coating shows the good performance in corrosion resistance. The coating prepared by this novel method show the great potential applications in different marine environments.

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Long-term Durability of Seawater Electrolysis for Hydrogen: From Catalysts to Systems

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Angewandte Chemie 2024年第47期136卷

作者： Yu Liu Yong Wang Prof. Paolo Fornasiero Prof. Ge Tian Prof. Peter Strasser Prof. Xiao-Yu Yang State Key Laboratory of Silicate Materials for Architectures & State Key Laboratory of Advanced Technology for Materials Synthesis and Processing & School of Chemistry Chemical Engineering and Life Sciences & Foshan Xianhu Laboratory & Laoshan Laboratory & School of Materials Science and Engineering & International School of Materials Science and Engineering Wuhan University of Technology Wuhan 430070 China Department of Chemical and Pharmaceutical Sciences University of Trieste and ICCOM-CNR and INSTM Trieste Research Units 34127 Trieste Italy Technical University Berlin Department of Chemistry 10623 Berlin Germany

Direct electrochemical seawater splitting is a renewable, scalab.e, and potentially economic approach for green hydrogen production in environments where ultra-pure water is not readily availab.e. However, issues related to low durability caused by complex ions in seawater pose great challenges for its industrialization. In this review, a mechanistic analysis of durability issues of electrolytic seawater splitting is discussed. We critically analyze the development of seawater electrolysis and identify the durability challenges at both the anode and cathode. Particular emphasis is given to elucidating rational strategies for designing electrocatalysts/electrodes/interfaces with long lifetimes in realistic seawater including inducing passivating anion layers, preferential OH − adsorption, employing anti-corrosion materials, fabricating protective layers, immobilizing Cl − on the surface of electrocatalysts, tailoring Cl − adsorption sites, inhibition of OH − binding to Mg 2+ and Ca 2+ , inhibition of Mg and Ca hydroxide precipitation adherence, and co-electrosynthesis of nano-sized Mg hydroxides. synthesis methods of electrocatalysts/electrodes and innovations in electrolyzer are also discussed. Furthermore, the prospects for developing seawater splitting technologies for clean hydrogen generation are summarized. We found that researchers have rethought the role of Cl − ions, as well as more attention to cathodic reaction and electrolyzers, which is conducive to accelerate the commercialization of seawater electrolysis.

关键词： direct electrochemical seawater splitting hydrogen production durability electrocatalysts/electrodes/interfaces design electrolyzer innovation

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Rapid fabrication and thermoelectric performance of SnTe via non-equilibrium laser 3D printing

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Rare Metals 2018年第4期37卷 300-307页

作者： Tian-Le Chen Chuang Luo Yong-Gao Yan Ji-Hui Yang Qing-Jie Zhang Ctirad Uher Xin-Feng Tang State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Department of Materials Science and Engineering University of Washington Department of Physics University of Michigan

Thermoelectric technologies based on Seebeck and Peltier effects, as energy techniques able to directly convert heat into electricity and vice versa, hold promise for addressing the global energy and environmental problems. The development of efficient and low-cost thermo- electric modules is the key to their large-scale commercial applications. In this paper, using a non-equilibrium laser 3D printing technique, we focus an attention on the fabrication of mid-temperature p-type SnTe thermoelectric materials. The influence of laser power, scanning speed and layer thickness on the macro-defects, chemical and phase composition, microstructure and thermoelectric performance was systematically investigated. First and foremost, the processing parameter window for printing a highquality layer is determined. This is followed by the finite element method used to simulate and verify the influence of the laser-induced molten pool temperature distribution on the final composition and microstructure. Finally, the high-performance SnTe layer with 10 mm × 10 mm in area is produced within seconds with room temperature Seebeck coefficient close to that of SnTe manufactured by the traditional methods. Consequently, this work lays a solid foundation for the future fabrication of thermoelectric modules using laser non-equilibrium printing techniques.

关键词： Selective laser melting Laser non-equilibriumheating SnTe compound Thermoelectric performance

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The role of grain boundary character on hydrogen energetics and kinetics in tungsten: Insights from atomic-scale modeling

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Acta Materialia 2025年

作者： Xue-Ru Zheng Xiang-Shan Kong C.S. Liu Xiao Zhou State Key Lab of Metal Matrix Composites School of Materials Science and Engineering Institute of Medical Robotics Shanghai Jiao Tong University Shanghai 200240 China Key Laboratory of Materials Physics Institute of Solid State Physics HFIPS Chinese Academy of Sciences Hefei 230031 China State key Laboratory of Advanced Equipment and Technology for Metal Forming and Key Laboratory for Liquid-Solid Structural Evolution and Processing of Materials (Ministry of Education) Shandong University Jinan Shandong 250061 China

Hydrogen (H) retention in tungsten (W), a critical challenge for its application as a plasma-facing material in nuclear reactors, is strongly influenced by grain boundaries (GBs). However, the precise role of GB in H diffusion and retention, as along with the intricate interactions with H energetics and kinetics, remains poorly understood and contentious yet. In this study, we conduct comprehensive atomistic simulations to explore the effects of GBs on H segregation, desorption, and diffusion in W. Our results reveal that GBs preferentially trap H, with the GB-H binding energies closely related to specific polyhedral structural units. We thoroughly analyze the migration pathways and energy barriers involved in H desorption, determining the critical desorption and decoupling temperatures using a statistical approach. More importantly, the rapid H diffusion channels are identified within GBs that contain discrete dislocation cores and pentagonal bipyramid (PBP) units. Based on these results, we propose a material design strategy that involves tuning GB types and temperature conditions to mitigate H retention. These findings provide essential insights into the energetics and kinetics of GB-H interactions, offering valuable guidance for the design of W-based materials with enhanced resistance to H retention through GB engineering.

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Influence of V/P Ratio on the Catalytic Performance of VPO/SiO_2 Catalysts for Ammoxidation of Chloro-Substituted Toluenes

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Wuhan University Journal of Natural Sciences 2019年第1期24卷 23-29页

作者： DONG Yanling XU Longlong ZHANG Zhenguo LIU Wenhui LI Xiongjian ZHONG Yalan HUANG Chi State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Tianhua Chemical Branch Xi'an Sunward Aeromat Co.Ltd. Sanjiang Chemical Factory of CSSG College of Chemistry and Molecular Sciences Wuhan University

A series of vanadium phosphate oxide(VPO) catalysts supported on silica(VPO/Si O2) with various mole ratios of V/P(nV:nP=1:0.8-1:3) were prepared through impregnation method. The catalytic activity was evaluated by ammoxidation reactions of several kinds of chloro-substituted toluenes(CT) in a fixed-bed reactor. The catalyst presented the best performance when nV:nP is 1:1.6. The prepared catalysts were characterized by N2 adsorption, hydrogen temperature programmed reduction(TPR) and ammonia temperature programmed desorption(TPD) and etc. The results reveal that P can decrease the bonding energy of V=O and increase the mobility of lattice oxygen which was beneficial for the improvement of the catalysts, while too much P can greatly decrease the average oxidation number of V which leads to deactivation of the catalysts. The surface acidity of the VPO/Si O2 catalysts is affected by nV:nP and the catalyst had the highest surface acidity when nV:nP is 1:1.6. The selectivity of catalysts is proportional to the surface acidity when nV:nP is lower than 1:3.0.

关键词： ammoxidation VPO/SiO2 catalyst substituted toluenes substituted benzonitriles

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Donor-Acceptor Molecule with Tict Character: A New Design Strategy for Organic Photothermal Material in Solar Energy

SSRN

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SSRN 2023年

作者： Wang, Chenguang Dai, Jianan Zhao, Meng Qi, Shuo Liu, Jing Jia, Tao Liu, Fangmeng Sun, Peng Li, Bo Zhou, Ji Lu, Geyu State Key Laboratory of Integrated Optoelectronics Key Laboratory of Advanced Gas Sensors of Jilin Province College of Electronic Science & Engineering Jilin University Changchun130012 China Key Laboratory of Forest Plant Ecology Ministry of Education Engineering Research Center of Forest Bio-Preparation College of Chemistry Chemical Engineering and Resource Utilization Northeast Forestry University Harbin150040 China Hebei Key Laboratory of Hazardous Chemicals Safety and Control Technology School of Chemical Safety North China Institute of Science and Technology Langfang065201 China State Kay Lab of New Ceramics and Fine Processing School of Materials Science and Engineering Tsinghua University Beijing100084 China International Center of Future Science Jilin University Changchun130012 China

Organic photothermal materials, particular the donor-acceptor (D-A) type ones, have attracted increased attention because they could efficiently transform solar energy to heat in an environmentally friendly manner. So far, there are many strategies to improve the fluorescence of D-A type molecules, while how to quench the fluorescence via non-radiative decay process and thus maximize the solar-thermal conversion efficiency is rarely investigated. Herein, a new design strategy is proposed to overcome this bottleneck, that is, formatting a unique twisted intramolecular charge-transfer (TICT) excitation state for the D-A type molecule. To demonstrate this new design strategy, three D-A molecules TPA-BTO, TPA-BTO-Py+ and GTPA-BTO-Py+ are synthesized with the consideration of employing stronger donor/acceptor moieties. The photophysical measurements and theoretical calculations reveal that these molecules display strong tendency to form TICT state, and the stronger donor/acceptor would significantly promote the TICT-based non-radiative decay process. Consequently, the target molecule GTPA-BTO-Py+ is totally non-fluorescent and could efficiently transform the absorbed solar energy to heat. Further combined with the wide absorption up to 1300 nm, GTPA-BTO-Py+ solid displays a high solar-thermal conversion efficiency of 20.5%. Finally, the utility of GTPA-BTO-Py+ as highly efficient photothermal material in solar energy is highlighted by water evaporation and thermoelectric generation. © 2023, The Authors. All rights reserved.

关键词： Molecules

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Enhanced performance of solid-state Li–O_2 battery using a novel integrated architecture of gel polymer electrolyte and nanoarray cathode

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Rare Metals 2018年第6期37卷 527-535页

作者： Liang Xiao Er-Wei Li Jing-Yu Yi Wen Meng Bo-Hua Deng Jin-Ping Liu School of Chemistry Chemical Engineering and Life Sciences Wuhan University of Technology State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology

The present work proposes a novel strategy to fabricate an integrated architecture of gel polymer electrolyte （GPE）-nanoarray cathode for lithium-O2 batteries （LOBs）. As a proof-of-concept experiment, the photo-initiated in situ polymerization of GPE was carried out via incorporating the precursor solution in advance into a self- standing binder-free oxygen electrode of Co3O4 nanosheets array grown on carbon cloth （Co3O4@CC）, forming an integrated GPE-Co3O4@CC architecture. The performance of the solid-state LOBs using the GPE-Co3O4@CC assembly is greatly enhanced compared to the counterparts with a traditional cell structure, in which GPE was sandwiched by a lithium metal and a cathode. The enhanced performance is ascribed to the combination of the in situ polymerization of GPE and the versatile structure of nanoarray electrode, which results in abundant interfacial contacts between GPE and electrode. This work presents an alternative way to develop high-performance solid-state LOBs by combining the advantages of both gel polymer electrolytes and nanoarray electrodes.

关键词： Solid-state Li-O2 battery Gel polymer electrolyte Co3O4 nanosheet Nanoarray electrode Electrolyte-cathode interface

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