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Intermediate phase-enhanced Ostwald ripening for the elimination of phase segregation in efficient inorganic CsPbIBr_(2)perovskite solar cells

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Science China materials 2021年第11期64卷 2655-2666页

作者： Wei Li Benjia Zhu Mathias Uller Rothmann Amelia Liu Weijian Chen Yen Yee Choo Narendra Pai Wenxin Mao Tian Zhang Qiaoliang Bao Xiaoming Wen Udo Bach Joanne Etheridge Yi-Bing Cheng Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory Xianhu hydrogen ValleyFoshan 528200China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China Department of Physics University of OxfordOxford OX13PUUnited Kingdom School of Physics and Astronomy Monash UniversityVictoria 3800Australia Centre for Micro-Photonics Swinburne University of TechnologyHawthorn 3122Australia Australian Research Council Centre of Excellence in Exciton Science Monash UniversityVictoria 3800Australia Department of Materials Science and Engineering Monash UniversityVictoria 3800Australia Department of Chemical Engineering Monash UniversityVictoria 3800Australia Commonwealth Scientific and Industrial Research Organization Manufacturing FlagshipClaytonVictoria 3168Australia Melbourne Centre for Nano fabrication 151 Wellington RoadClaytonVIC 3168Australia Monash Centre for Electron Microscopy Monash UniversityVictoria 3800Australia

Mixed halide perovskites with the ability to tune bandgaps exhibit attractive applications in tandem solar cells,building integrated photovoltaic and wavelength-tunable light-emitting ***,halide demixing under illumination or in the dark with a charge-carrier injection in both hybrid and inorganic perovskites results in bandgap instability and current-density-voltage(J-V)hysteresis,which can significantly hamper their ***,we demonstrate that halide segregation and J-V hysteresis in mixed halide inorganic CsPbIBr_(2)solar cells can be effectively mitigated by introducing an intermediate phase-enhanced Ostwald ripening through the control of the chemical composition in the CsPbIBr_(2)precursor *** amounts of either PbBr_(2)or CsI are incorporated into originally even molar amounts of PbBr_(2)and CsI precursor *** the PbBr_(2)-excess,we observed an enlarged perovskite grain size,no detectable halide phase segregation at the grain boundaries nor the perovskite/TiO2 interface,an increased minority carrier lifetime,a reduced J-V hysteresis,and an improved solar-cell ***,different CsI:PbBr_(2)stoichiometric ratios were found to have different effects on the performance of the perovskite solar *** excessive lead phase is reactive with the dimethyl sulfoxide(DMSO)in the precursor solution to form the Pb(I,Br)2·DMSO complex and the quasi-twodimensional(2D)CsPb_(2)(I,Br)5,which are conducive to Ostwald maturation and defect ***,the CsPbIBr_(2)solar cell with a PbBr_(2)-excess precursor composition reaches a power conversion efficiency(PCE)of 9.37%(stabilized PCE of 8.48%)and a maximum external quantum efficiency of over 90%.

关键词： solar cells phase segregation CsPbIBr_(2) cathodoluminescence transmission electron microscope

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Modulating charge transfer dynamics in one-dimensional covalent organic frameworks for boosted photocatalytic H 2 generation

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Journal of Catalysis 2025年 450卷

作者： Ruxue Wang Zhongliao Wang Lingling Li Lijie Zhang Jinfeng Zhang Huile Jin Quanlong Xu Yuechang Wei Yun Yang Shun Wang Wenzhou Key Lab of Advanced Energy Storage and Conversion Zhejiang International Joint Laboratory of Optical Functional Materials College of Chemistry and Materials Engineering Wenzhou University Wenzhou 325027 China Anhui Key Laboratory of Energetic Materials College of Physics and Electronic Information Huaibei Normal University Anhui 235000 China School of Material Science and Technology Jilin Institute of Chemical Technology Jilin 132022 China State Key Laboratory of Heavy Oil Processing Key Laboratory of Optical Detection Technology for Oil and Gas College of Science China University of Petroleum Beijing 102249 China

Achieving strong dipole moment has been established as a promising strategy to improve the charge separation of nitrogen (N)-heterocycle-based covalent organic frameworks (COFs). However, the intrinsic polarization property causes weak π-electron delocalization and detrimentally affects the photocatalytic solar fuel generation. Herein, N-heterocycle-functionalized nonlinear C 2 linkage with nonuniform N atom distribution was condensed with planar C 4 knots to construct one-dimensional (1D) COFs, which possesses strong dipole moment, thus contributing efficient exciton dissociation and high charge carrier separation feature. Furthermore, a fully π-conjugated segment was simultaneously formed, serving as fast charge carrier transfer channel. As a result, the synthesized 1D COFs achieves a remarkable photocatalytic H 2 generation performance, and the aquantum efficiency (AQE) was detected to be 0.17 % at 420 nm. This work provides a general protocol for precisely modulating COF structure at molecular level to achieve high photocatalytic performance.

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Liquid Fluxional Ga Single Atom Catalysts for Efficient Electrochemical CO2Reduction

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Angewandte Chemie 2022年第3期135卷

作者： Dr. Zedong Zhang Jiexin Zhu Dr. Shenghua Chen Prof. Wenming Sun Prof. Dingsheng Wang Department of Chemistry Tsinghua University Beijing 100084 China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 Hubei China Department of Chemistry Beijing Key Laboratory for Optical Materials and Photonic Devices Capital Normal University Beijing 100048 China

Precise design and tuning of the micro-atomic structure of single atom catalysts (SACs) can help efficiently adapt complex catalytic systems. Herein, we inventively found that when the active center of the main group element gallium (Ga) is downsized to the atomic level, whose characteristic has significant differences from conventional bulk and rigid Ga catalysts. The Ga SACs with a P, S atomic coordination environment display specific flow properties, showing CO products with FE of ≈92 % at −0.3 V vs. RHE in electrochemical CO 2 reduction (CO 2 RR). Theoretical simulations demonstrate that the adaptive dynamic transition of Ga optimizes the adsorption energy of the *COOH intermediate and renews the active sites in time, leading to excellent CO 2 RR selectivity and stability. This liquid single atom catalysts system with dynamic interfaces lays the foundation for future exploration of synthesis and catalysis.

关键词： CO2RR Fluxional Single Atom Catalysts Liquid Metal Ga

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Abatement of Emissions of a Residential Wood Stove: Effect of the Catalyst on Gaseous and Condensable Pollutants Concentration and Their Toxicity

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ACS Omega 2025年第24期10卷 25506-25517页

作者： Marvin lab.ureur Maxence Hannard Tarek Barakat Abhishek Goel Jordi Cornette Svend Bram Patricia Renard Thomas Duquesne Bao-Lian Su Laboratory of Inorganic Materials Chemistry (CMI) − Namur Institute of Structured Matter (NISM) University of Namur rue de Bruxelles 61 Namur 5000 Belgium；Stuv S.A. Rue Riverre 10-12 Floreffe 5150 Belgium Laboratory of Inorganic Materials Chemistry (CMI) − Namur Institute of Structured Matter (NISM) University of Namur rue de Bruxelles 61 Namur 5000 Belgium；Empa - Swiss Federal Laboratories for Materials Science and Technology Ueberlandstrasse 129 Dübendorf 8600 Switzerland Thermo and Fluid Dynamics (FLOW) Vrije Universiteit Brussel (VUB) Pleinlaan 2 Brussels 1050 Belgium；Brussels Institute for Thermal-fluid Systems and Clean Energy (BRITE) Vrije Universiteit Brussel (VUB) and Université Libre de Bruxelles (ULB) Brussels 1050 Belgium Thermo and Fluid Dynamics (FLOW) Vrije Universiteit Brussel (VUB) Pleinlaan 2 Brussels 1050 Belgium；Brussels Institute for Thermal-fluid Systems and Clean Energy (BRITE) Vrije Universiteit Brussel (VUB) and Université Libre de Bruxelles (ULB) Brussels 1050 Belgium；Faculty of Aerospace Engineering Delft University of Technology Kluyverweg 1 Delft 2629 HS The Netherlands Laboratory of Biochemistry and Cell Biology (URBC)-Namur Research Institute for Life Sciences (NARILIS) University of Namur Rue de Bruxelles 61 Namur 5000 Belgium Stuv S.A. Rue Riverre 10-12 Floreffe 5150 Belgium Laboratory of Inorganic Materials Chemistry (CMI) − Namur Institute of Structured Matter (NISM) University of Namur rue de Bruxelles 61 Namur 5000 Belgium；State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology 122 Hongshan Luoshi Road Wuhan 430070 China

The use of biomass combustion for residential heating purposes is crucial for reaching the European Union’s 2050 climate-neutrality goals. It, however, raises environmental and health concerns. This study explores the impact of a patented catalyst on wood stove emissions and, notably, its influence on cytotoxicity by comparing flue gas composition with and without the catalyst. Organic gaseous compounds (OGC) generated by wood combustion comprise two subgroups: water-soluble condensable organic compounds (WSCOC) and high-saturating vapor organic compounds (HSVOC). The second is mainly composed of methane, a molecule challenging to oxidize into CO2at these operating temperatures. While the catalyst moderately eliminates OGC (19%) in general, it excels in removing CO (87%) and WSCOC (80%), particularly polycyclic aromatic hydrocarbons (PAH) (91%). Bioassays on the A549 human cell line show that the catalytic WSCOC removal is correlated with a significant decrease in cytotoxicity (50%). Additionally, particle number size distribution measurements suggest that the catalyst facilitates the deposition of particles larger than 10 μm, leading to a 66% reduction in the particulate mass concentration. These results underscore the catalyst’s role in mitigating harmful gaseous emissions and reducing the health risks associated with wood stove use, particularly by targeting toxic WSCOC.

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High-Entropy Lithium Argyrodite Solid Electrolytes Enabling Stable All-Solid-state Batteries

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Angewandte Chemie 2023年第50期135卷

作者： Shenghao Li Jing Lin Mareen Schaller Sylvio Indris Xin Zhang Torsten Brezesinski Ce-Wen Nan Shuo Wang Florian Strauss Center of Smart Materials and Devices State Key Laboratory of Advanced Technology for Materials Synthesis and Processing & School of Material Science and Engineering Wuhan University of Technology Wuhan 430070 China Institute of Nanotechnology Karlsruhe Institute of Technology (KIT) Hermann-von-Helmholtz-Platz 1 76344 Eggenstein-Leopoldshafen Germany Institute for Applied Materials-Energy Storage Systems (IAM-ESS) Karlsruhe Institute of Technology (KIT) Hermann-von-Helmholtz-Platz 1 76344 Eggenstein-Leopoldshafen Germany State Key Laboratory of New Ceramics and Fine Processing School of Materials Science and Engineering Tsinghua University Beijing 100084 China Foshan (Southern China) Institute for New Materials Foshan 528200 China

Superionic solid electrolytes (SEs) are essential for bulk-type solid-state battery (SSB) applications. Multicomponent SEs are recently attracting attention for their favorable charge-transport properties, however a thorough understanding of how configurational entropy (Δ S conf ) affects ionic conductivity is lacking. Here, we successfully synthesized a series of halogen-rich lithium argyrodites with the general formula Li 5.5 PS 4.5 Cl x Br 1.5- x (0≤ x ≤1.5). Using neutron powder diffraction and 31 P magic-angle spinning nuclear magnetic resonance spectroscopy, the S 2− /Cl − /Br − occupancy on the anion sublattice was quantitatively analyzed. We show that disorder positively affects Li-ion dynamics, leading to a room-temperature ionic conductivity of 22.7 mS cm −1 (9.6 mS cm −1 in cold-pressed state) for Li 5.5 PS 4.5 Cl 0.8 Br 0.7 (Δ S conf =1.98 R ). To the best of our knowledge, this is the first experimental evidence that configurational entropy of the anion sublattice correlates with ion mobility. Our results indicate the possibility of improving ionic conductivity in ceramic ion conductors by tailoring the degree of compositional complexity. Moreover, the Li 5.5 PS 4.5 Cl 0.8 Br 0.7 SE allowed for stable cycling of single-crystal LiNi 0.9 Co 0.06 Mn 0.04 O 2 (s-NCM90) composite cathodes in SSB cells, emphasizing that dual-substituted lithium argyrodites hold great promise in enabling high-performance electrochemical energy storage.

关键词： Argyrodite High-Entropy materials Solid Electrolyte Solid-state Batteries

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A TiSe 2 -Graphite Dual Ion Battery: Fast Na-Ion Insertion and Excellent Stability

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Angewandte Chemie (International ed. in English) 2021年第34期60卷 18430-18437页

作者： Runtian Zheng Haoxiang Yu Xikun Zhang Yang Ding Maoting Xia Kangzhe Cao Jie Shu Alexandru Vlad Bao-Lian Su School of Materials Science and Chemical Engineering Ningbo University Ningbo 315211 Zhejiang China. Laboratory of Inorganic Materials Chemistry (CMI) University of Namur 61 rue de Bruxelles 5000 Namur Belgium. State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 Hubei China. Henan Province Key Laboratory of Utilization of Non-Metallic Mineral in the South of Henan Xinyang Normal University Xinyang 464000 Henan China. Institute of Condensed Matter and Nanosciences Université Catholique de Louvain Place Louis Pasteur 1L4.01.02 1348 Louvain-la-Neuve Belgium.

The sodium dual ion battery (Na-DIB) technology is proposed as highly promising alternative over lithium-ion batteries for the stationary electrochemical energy-storage devices. However, the sluggish reaction kinetics of anode materials seriously impedes their practical implementation. Herein, a Na-DIB based on TiSe -graphite is reported. The high diffusion coefficient of Na-ions (3.21×10 -1.20×10 cm s ) and the very low Na-ion diffusion barrier (0.50 eV) lead to very fast electrode kinetics, alike in conventional surface capacitive storage systems. In-situ investigations reveal that the fast Na-ion diffusion involves four insertion stage compositions. A prototype cell shows a reversible capacity of 81.8 mAh g at current density of 100 mA g , excellent stability with 83.52 % capacity retention over 200 cycles and excellent rate performance, suggesting its potential for next-generation large scale high-performance stationary energy storage systems.

关键词： TiSe2 dual-ion batteries graphite cathodes reaction mechanisms sodium

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无模板法合成具有增强催化活性的分级纳米孔结构MIL-101(Cr)

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中国科学：材料科学（英文版） 2021年第1期64卷 252-258页

作者：赵田李松贺肖宇轩 Christoph Janiak 常刚刚田歌阳晓宇 State Key Laboratory of Advanced Technology for Materials Synthesis and Processing & School of Materials Science and Engineering & School of Chemistry Chemical Engineering and Life Science Wuhan University of Technology Wuhan 430070 China Key Laboratory of Advanced Packaging Materials and Technology of Hunan Province School of Packaging and Materials Engineering Hunan University of Technology Zhuzhou 412007 China Institut für Anorganische Chemie und Strukturchemie Universität Düsseldorf Universitätsstr. 1 D-40225 Düsseldorf Germany Southern Marine Science and Engineering Guangdong Laboratory (Zhuhai) & School of Chemical Engineering and Technology Sun Yat-sen University Zhuhai 519000 China School of Engineering and Applied Sciences Harvard University Cambridge Massachusetts 02138 USA

MIL-101(Cr)是最重要的金属有机框架(MOFs)材料之一,稳定的框架结构和超高的比表面积使其在众多科学领域得到了广泛研究和应用.但是MIL-101(Cr)的合成条件比较苛刻,且稳定性较强,因此,有关于其分级结构的研究报道仍比较少.本文提出了一... 详细信息

MIL-101(Cr)是最重要的金属有机框架(MOFs)材料之一,稳定的框架结构和超高的比表面积使其在众多科学领域得到了广泛研究和应用.但是MIL-101(Cr)的合成条件比较苛刻,且稳定性较强,因此,有关于其分级结构的研究报道仍比较少.本文提出了一种简单制备分级纳米孔结构MIL-101(Cr)的方法,即以乙酸作为调节剂,采用水热合成的方法,一步得到具有微孔-介孔-大孔分级结构的MIL-101(Cr)材料.实验结果表明,该分级结构的MIL-101(Cr)与无分级结构的MIL-101(Cr)相比,其大分子染料吸附能力和催化能力均有显著提高.而且分级结构MIL-101(Cr)负载了磷钨酸催化剂之后,表现出了与均相催化剂(纯磷钨酸)相当的催化能力.进一步研究发现,使用其他短碳链的一元羧酸作为调节剂,如丙酸、丁酸等,也可获得类似分级纳米结构MIL-101(Cr).

关键词： Template-free synthesis micro-meso-macroporous hierarchy MIL-101(Cr)

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Doping-induced phase transition based on low-temperature molten salt template method to design self-growing and high-active electrocatalysts for water splitting

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Applied Surface Science 2025年 709卷

作者： Junlong Liu Chuanhua Li Manyi Chen Wei Xiao Shenghua Zhu Peng Lv Xuemin Yan College of Chemistry and Environmental Engineering Yangtze University Jingzhou 434023 Hubei PR China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 PR China State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering Ningxia University Yinchuan 750021 PR China Hubei Engineering Research Centers for Clean Production and Pollution Control of Oil and Gas Fields Yangtze University Jingzhou 434023 Hubei PR China

Transition metal sulfides have attracted much attention in environmentally friendly hydrogen evolution via water electrolysis because they can improve the kinetic process. In this work, self-growing chromium (Cr) doped nickel sulfide on nickel foam (Cr-NiS/NF) was synthesized by low-temperature molten salt method lacking binder and non-reactive gas protection. The structural analyses verified that active material was transformed from NiS (R3m) and Ni 3 S 2 into NiS (R3m) and NiS (P63/mmc) by Cr doping-induced phase transition. Furthermore, Cr-NiS/NF consisting of NiS (R3m) and NiS (P63/mmc) shows more excellent catalytic performance compared with NiS@Ni 3 S 2 /NF consisting of NiS (R3m) and Ni 3 S 2 . For oxygen evolution reaction (OER), Cr-NiS/NF reaches 100 mA cm −2 with overpotential of 220 mV, and reaches 50 mA cm −2 with overpotential of 243 mV for hydrogen evolution reaction (HER). Simultaneously, it is employed in a dual-electrode water electrolysis setup, attaining cell voltage of 1.51 V at 10 mA cm −2 . In addition, density functional theory (DFT) calculation reveals that Cr doping-induced new phase can enhance the catalytic performance, aligning well with the experimental observations. Meanwhile, doping induced pre-catalysts undergo different surface reconstructions. The surface reconstruction of NiS@Ni 3 S 2 /NF yields Ni(OH) 2 , and that of Cr-NiS/NF yields NiOOH. Therefore, this research offers a novel and practical approach, along with theoretical insights, for developing cost-effective yet highly efficient electrocatalysts.

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The Role of the Molecular Encapsulation Effect in Stabilizing Hydrogen-Bond-Rich Gel-state Lithium Metal Batteries

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Angewandte Chemie 2024年第27期136卷

作者： Hantao Xu Wei Deng Lei Shi Juncai Long Yongcai Zhang Prof. Lin Xu Prof. Liqiang Mai State Key Laboratory of Advanced Technology for Materials Synthesis and Processing School of Materials Science and Engineering Wuhan University of Technology Wuhan 430070 P.R. China School of Chemistry and Chemical Engineering Yangzhou University Yangzhou 225009 P.R. China Hubei Longzhong Laboratory Wuhan University of Technology (Xiangyang Demonstration Zone) Xiangyang 441000 Hubei P.R. China Hainan Institute Wuhan University of Technology Sanya 572000 P.R. China

Gel-state polymer electrolytes with superior mechanical properties, self-healing abilities and high Li + transference numbers can be obtained by in situ polymerization of monomers with hydrogen-bonding moieties. However, it is overlooked that the active hydrogen atoms in hydrogen-bond donors experience displacement reactions with lithium metal in lithium metal batteries (LMBs), leading to corrosion of the lithium metal. Herein, it is discovered that the addition of hydrogen-bond acceptors to hydrogen-bond-rich gel-state electrolytes modulates the chemical activity of the active hydrogen atoms via the formation of hydrogen-bonded intermolecular interactions. The characterizations reveal that the added hydrogen-bond acceptors encapsulate the active hydrogen atoms to suppress the interfacial chemical corrosions of lithium metals, thereby enhancing the chemical stability of the polymer structure and interphase. With the employment of this strategy, a 1.1 Ah LiNi 0.8 Co 0.1 Mn 0.1 O 2 /Li metal pouch cell achieves stable cycling with 96.3 % capacity retention at 100 cycles. This new approach indicates a feasible path for achieving in situ polymerization of highly stable gel-state-based LMBs.

关键词： in situ polymerization molecular encapsulation effect interfaces lithium metal batteries gel-state polymer electrolytes

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Sym- andAsym-Expanded Heterohelicene Isomers Featuring Extended Multi-Resonance Skeleton for Narrowband Deep-Blue Fluorescence

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Angewandte Chemie 2025年

作者： Dr. Xuan Zeng Xiaofeng Luo Dr. Guoyun Meng Prof. Xuewen Wang Dr. Dongdong Zhang Prof. Lian Duan School of Chemistry Chemical Engineering and Life Science State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 P. R. China Key Lab of Organic Optoelectronics and Molecular Engineering of Ministry of Education Department of Chemistry Tsinghua University Beijing 100084 P. R. China These authors contributed equally to this work Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory Xianhu hydrogen Valley Foshan 528200 P. R. China Center for Flexible Electronics Technology Tsinghua University Beijing 100084 P. R. China

Expanded heterohelicenes composed of alternating linearly and angularly fused multi-resonance (MR) skeletons have gained wide interest owing to their promising narrowband emissions. Herein, a pair of sym - and asym -expanded heterohelicene isomers was obtained by merging boron/oxygen (B/O)-embedded MR triangulene and indolo[3,2,1- jk ]carbazole units via one-pot synthesis. Owing to their fully resonating extended helical skeleton, the target heterohelicenes exhibit a significantly narrowed spectra bandwidth while emission red-shifting, thus affording deep-blue narrowband emission with a peak at approximately 460 nm, full-width-at-half-maximum (FWHM) of only 18 nm, and near-unity photoluminescence quantum yields. In comparison to the symmetrical structure, the asym -expanded heterohelicene displays suppressed aggregation within doped films, thereby showing superior narrowband electroluminescence in devices with CIE coordinates of (0.12, 0.18) and a high external quantum efficiency of up to 25 %, which retains 18.1 % even at a high luminance of 10,000 cd m −1 . Overall, this work provides a novel paradigm for the development of narrowband expanded heterohelicenes.

关键词： multiple resonance expanded helicene asymmetrical heterohelicene narrowband emission spectral broadening

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