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Triple-function Hydrated Eutectic Electrolyte for Enhanced Aqueous Zinc Batteries

Angewandte Chemie 2023年第40期135卷

作者： Yunpeng Zhong Xuesong Xie Prof. Zhiyuan Zeng Prof. Bingan Lu Prof. Gen Chen Prof. Jiang Zhou School of Materials Science and Engineering Hunan Provincial Key Laboratory of Electronic Packaging and Advanced Functional Materials Central South University Changsha Hunan 410083 P. R. China Contribution: Conceptualization (equal) Data curation (lead) Formal analysis (lead) Investigation (equal) Methodology (lead) Writing - original draft (lead) Contribution: Formal analysis (supporting) Investigation (supporting) Validation (lead) Writing - review & editing (supporting) Department of Materials Science and Engineering City University of Hong Kong 83 Tat Chee Avenue Kowloon Hong Kong 999077 P. R. China Contribution: Formal analysis (supporting) Investigation (supporting) Writing - review & editing (supporting) School of Physics and Electronics Hunan University Changsha Hunan 410082 P. R. China Contribution: Data curation (supporting) Investigation (supporting) Writing - review & editing (supporting) Contribution: Conceptualization (equal) Formal analysis (supporting) Funding acquisition (supporting) Resources (lead) Supervision (equal) Validation (lead) Writing - review & editing (equal) Contribution: Conceptualization (equal) Funding acquisition (lead) Investigation (equal) Project administration (lead) Supervision (equal) Writing - review & editing (equal)

Aqueous rechargeable zinc-ion batteries (ARZBs) are impeded by the mutual problems of unstable cathode, electrolyte parasitic reactions, and dendritic growth of zinc (Zn) anode. Herein, a triple-functional strategy by introducing the tetramethylene sulfone (TMS) to form a hydrated eutectic electrolyte is reported to ameliorate these issues. The activity of H 2 O is inhibited by reconstructing hydrogen bonds due to the strong interaction between TMS and H 2 O. Meanwhile, the preferentially adsorbed TMS on the Zn surface increases the thickness of double electric layer (EDL) structure, which provides a shielding buffer layer to suppress dendrite growth. Interestingly, TMS modulates the primary solvation shell of Zn 2+ ultimately to achieve a novel solvent co-intercalation ((Zn-TMS) 2+ ) mechanism, and the intercalated TMS works as a “pillar” that provides more zincophilic sites and stabilizes the structure of cathode (NH 4 V 4 O 10 , (NVO)). Consequently, the Zn||NVO battery exhibits a remarkably high specific capacity of 515.6 mAh g −1 at a low current density of 0.2 A g −1 for over 40 days. This multi-functional electrolytes and solvent co-intercalation mechanism will significantly propel the practical development of aqueous batteries.

关键词： Double Electric Layer Electrochemistry Eutectic Electrolyte Hydrogen Bond Network Zinc Battery

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Universal Sub-Nanoreactor Strategy for Synthesis of Yolk-Shell MoS2Supported Single Atom Electrocatalysts toward Robust Hydrogen Evolution Reaction

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Angewandte Chemie 2023年第40期135卷

作者： Feilong Gong Yuheng Liu Yang Zhao Prof. Wei Liu Prof. Guang Zeng Prof. Guoqing Wang Prof. Yonghui Zhang Lihua Gong Prof. Jian Liu Key Laboratory of Surface and Interface Science and Technology of Henan Province College of Material and Chemical Engineering Zhengzhou University of Light Industry Zhengzhou Henan 450001 P. R. China Contribution: Conceptualization (equal) Formal analysis (equal) Funding acquisition (lead) Investigation (lead) Visualization (equal) Writing - original draft (lead) Contribution: Data curation (lead) Formal analysis (equal) Investigation (equal) Validation (equal) Visualization (equal) State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian Liaoning 116023 P. R. China Contribution: Data curation (equal) Formal analysis (equal) Resources (equal) Validation (equal) Visualization (equal) Contribution: Data curation (equal) Formal analysis (equal) Investigation (equal) Contribution: Data curation (equal) Methodology (equal) Software (equal) Validation (equal) Contribution: Formal analysis (equal) Software (equal) Writing - review & editing (equal) Contribution: Conceptualization (equal) Data curation (equal) Formal analysis (lead) Software (lead) Writing - review & editing (equal) DICP-Surrey Joint Centre for Future Materials Department of Chemical and Process Engineering and Advanced Technology Institute of University of Surrey Guildford Surrey GU2 7XH UK College of Chemistry and Chemical Engineering Inner Mongolia University Hohhot Inner Mongolia 010021 P. R. China Contribution: Conceptualization (lead) Formal analysis (equal) Funding acquisition (equal) Project administration (lead) Supervision (lead) Writing - review & editing (lead)

The coordination structure determines the electrocatalytic performances of single atom catalysts (SACs), while it remains a challenge to precisely regulate their spatial location and coordination environment. Herein, we report a universal sub-nanoreactor strategy for synthesis of yolk-shell MoS 2 supported single atom electrocatalysts with dual-anchored microenvironment of vacancy-enriched MoS 2 and intercalation carbon toward robust hydrogen-evolution reaction. Theoretical calculations reveal that the “E-Lock” and “E-Channel” are conducive to stabilize and activate metal single atoms. A group of SACs is subsequently produced with the assistance of sulfur vacancy and intercalation carbon in the yolk-shell sub-nanoreactor. The optimized C−Co−MoS 2 yields the lowest overpotential (η 10 =17 mV) compared with previously reported MoS 2 -based electrocatalysts to date, and also affords a 5–9 fold improvement in activity even comparing with those as-prepared single-anchored analogues. Theoretical results and in situ characterizations unveil its active center and durability. This work provides a universal pathway to design efficient catalysts for electro-refinery.

关键词： Electrocatalyst Nanostructures Sub-Nanoreactor Universal Strategy Water Splitting

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Carbazole-Dendronized Luminescent Radicals

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Angewandte Chemie 2023年第28期135卷

作者： Rui Xiaotian Wataru Ota Prof. Tohru Sato Minori Furukori Prof. Yasuo Nakayama Prof. Takuya Hosokai Eri Hisamura Kazuhiro Nakamura Kenshiro Matsuda Dr. Kohei Nakao Prof. Andrew P. Monkman Prof. Ken Albrecht Department of Applied Science for Electronics and Materials Interdisciplinary Graduate School of Engineering Sciences Kyushu University 6-1 Kasuga-Koen Kasuga-shi Fukuoka 816-8580 Japan Contribution: Conceptualization (supporting) Data curation (lead) Formal analysis (lead) Funding acquisition (supporting) Investigation (equal) Visualization (equal) Writing - original draft (lead) MOLFEX Inc. Takano Nishibiraki-cho 34–4 Sakyo-ku Kyoto 606-8103 Japan Contribution: Conceptualization (supporting) Data curation (equal) Formal analysis (equal) Investigation (equal) Methodology (equal) Resources (supporting) Software (supporting) Visualization (supporting) Writing - original draft (supporting) Fukui Institute for Fundamental Chemistry Kyoto University Takano Nishibiraki-cho 34–4 Sakyo-ku Kyoto 606-8103 Japan Department of Molecular Engineering Graduate School of Engineering Kyoto University Nishikyo-ku Kyoto 615-8510 Japan Elements Strategy Initiative for Catalysts & Batteries (ESICB) Kyoto University Kyotodaigaku Katsura Nishikyo-ku Kyoto 615-8245 Japan Contribution: Conceptualization (supporting) Software (supporting) Supervision (equal) Validation (supporting) Writing - review & editing (supporting) Department of Pure and Applied Chemistry Graduate School of Science and Technology Tokyo University of Science 2641 Yamazaki Noda Chiba 278-8510 Japan National Institute of Advanced Industrial Science and Technology (AIST) Tsukuba Central 5 1-1-1 Higashi Tsukuba Ibaraki 305-8565 Japan Contribution: Data curation (supporting) Formal analysis (supporting) Investigation (supporting) Contribution: Supervision (supporting) Writing - review & editing (supporting) Contribution: Conceptualization (supporting) Data curation (supporting) Formal analysis (supporting) Funding acquisition (supporting) Supervision (equal) Writing - review & editing (equal) Institute for Materials Chemistry and Engineering Kyushu University 6-1 Kasuga-Koen Kasuga-shi Fukuoka 816-8580 J

A series of carbazole-dendronized tris(2,4,6-trichlorophenyl)methyl (TTM) radicals have been synthesized. The photophysical properties of dendronized radicals up to the fourth generation were compared systematically to understand how structure–property relationships evolve with generation. The photoluminescence quantum yield (PLQY) was found to increase with the increasing generation, and the fourth generation (G4TTM) in cyclohexane solution showed a PLQY as high as 63 % at a wavelength of 627 nm (in the deep-red region) from the doublet state. The dendron modification strategy also showed a blue-shift of the emission on increasing the generation number, and the photostability was also increased compared to the bare TTM radical.

关键词： Carbazoles Dendrimers Excited Doublet State Luminescencent Materials Stable Radicals

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Extending the π-Conjugated System in Spiro-Type Hole Transport Material Enhances the Efficiency and Stability of Perovskite Solar Modules

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Angewandte Chemie 2023年第29期135卷

作者： Xuepeng Liu Bin Ding Mingyuan Han Zhenhai Yang Jianlin Chen Pengju Shi Xiangying Xue Rahim Ghadari Xianfu Zhang Rui Wang Keith Brooks Li Tao Sachin Kinge Songyuan Dai Jiang Sheng Paul J. Dyson Mohammad Khaja Nazeeruddin Yong Ding Beijing Key Laboratory of Novel Thin-Film Solar Cells School of New Energy North China Electric Power University Beijing 102206 P. R. China Contribution: Investigation (lead) Institute of Chemical Sciences and Engineering École Polytechnique Fédérale de Lausanne (EPFL) 1015 Lausanne Switzerland Contribution: Methodology (lead) Contribution: Methodology (equal) Ningbo Institute of Materials Technology and Engineering Chinese Academy of Sciences (CAS) Ningbo 315201 China Contribution: Data curation (equal) Contribution: Validation (equal) School of Engineering Westlake University Hangzhou 310024 China Contribution: Formal analysis (equal) Contribution: Investigation (equal) Computational Chemistry Laboratory Department of Organic and Biochemistry Faculty of Chemistry University of Tabriz Tabriz *** Iran Contribution: Software (lead) Contribution: Visualization (equal) School of Microelectronic & Faculty of Physics and Electronic Science Hubei University Wuhan 430062 China Toyota Motor Europe Toyota Motor Technical Centre Advanced Technology Div. Hoge Wei 33 1930 Zaventum Belgium Contribution: Resources (equal) Contribution: Supervision (equal) Contribution: Writing - original draft (equal) Writing - review & editing (equal) Contribution: Conceptualization (equal) Writing - original draft (equal) Writing - review & editing (equal) Contribution: Supervision (equal) Writing - original draft (lead)

Hole transport materials (HTMs) are a key component of perovskite solar cells (PSCs). The small molecular 2,2′,7,7′-tetrakis(N,N-di-p-methoxyphenyl)-amine-9,9′-spirobifluorene (spiro-OMeTAD, termed “Spiro”) is the most successful HTM used in PSCs, but its versatility is imperfect. To improve its performance, we developed a novel spiro-type HTM (termed “DP”) by substituting four anisole units on Spiro with 4-methoxybiphenyl moieties. By extending the π-conjugation of Spiro in this way, the HOMO level of the HTM matches well with the perovskite valence band, enhancing hole mobility and increasing the glass transition temperature. DP-based PSC achieves high power conversion efficiencies (PCEs) of 25.24 % for small-area (0.06 cm 2 ) devices and 21.86 % for modules (designated area of 27.56 cm 2 ), along with the certified efficiency of 21.78 % on a designated area of 27.86 cm 2 . The encapsulated DP-based devices maintain 95.1 % of the initial performance under ISOS-L-1 conditions after 2560 hours and 87 % at the ISOS-L-3 conditions over 600 hours.

关键词： Hole Transport Materials Modules Perovskite Solar Cells π-Conjugated System Stability

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100 essential questions for the future of agriculture

Modern Agriculture

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Modern Agriculture 2023年第1期1卷

作者： Yuming Hu Taolan Zhao Yafang Guo Meng Wang Kerstin Brachhold Chengcai Chu Andrew Hanson Sachin Kumar Rongcheng Lin Wenjin Long Ming Luo Jian Feng Ma Yansong Miao Shaoping Nie Yu Sheng Weiming Shi James Whelan Qingyu Wu Ziping Wu Wei Xie Yinong Yang Chao Zhao Lei Lei Yong-Guan Zhu Qifa Zhang Wiley-VCH GmbH Weinheim Germany Contribution: Conceptualization (equal) Data curation (equal) Formal analysis (equal) Investigation (equal) Methodology (equal) Project administration (equal) Writing - original draft (equal) Writing - review & editing (equal) Contribution: Investigation (equal) Resources (equal) Writing - original draft (equal) Contribution: Data curation (equal) Investigation (equal) Visualization (equal) Contribution: Writing - review & editing (equal) State Key Laboratory for Conservation and Utilization of Subtropical Agro-Bioresources College of Agriculture South China Agricultural University Guangzhou China Contribution: Investigation (equal) Resources (equal) Horticultural Sciences Department University of Florida Gainesville Florida USA Rumen Biotechnology Laboratory Animal Nutrition Division ICAR-National Dairy Research Institute Karnal Haryana India Key Laboratory of Photobiology Institute of Botany Chinese Academy of Sciences Beijing China School of Economics and Management China Agricultural University Beijing China Guangdong Provincial Key Laboratory of Applied Botany & Agriculture and Biotechnology Research Center South China Botanical Garden Chinese Academy of Sciences Guangzhou China Institute of Plant Science and Resources Okayama University Kurashiki Japan School of Biological Sciences Nanyang Technological University Singapore City Singapore State Key Laboratory of Food Science and Technology China-Canada Joint Lab of Food Science and Technology (Nanchang) Nanchang University Nanchang China China Center for Agricultural Policy School of Advanced Agricultural Sciences Peking University Beijing China State Key Laboratory of Soil and Sustainable Agriculture Institute of Soil Science Chinese Academy of Sciences Nanjing China State Key Laboratory of Plant Physiology and Biochemistry College of Life Sciences Zhejiang University Hangzhou Zhejiang China Department of Animal Plant and Soil Sciences La Trobe University Me

The world is at a crossroad when it comes to agriculture. The global population is growing, and the demand for food is increasing, putting a strain on our agricultural resources and practices. To address this challenge, innovative, sustainable, and inclusive approaches to agriculture are urgently required. In this paper, we launched a call for Essential Questions for the Future of Agriculture and identified a priority list of 100 questions. We focus on 10 primary themes: transforming agri-food systems, enhancing resilience of agriculture to climate change, mitigating climate change through agriculture, exploring resources and technologies for breeding, advancing cultivation methods, sustaining healthy agroecosystems, enabling smart and controlled-environment agriculture for food security, promoting health and nutrition-driven agriculture, exploring economic opportunities and addressing social challenges, and integrating one health and modern agriculture. We emphasise the critical importance of interdisciplinary and multidisciplinary research that integrates both basic and applied sciences and bridges the gaps among various stakeholders for achieving sustainable agriculture.

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A Universal Molten Salt Method for Direct Upcycling of Spent Ni-rich Cathode towards Single-crystalline Li-rich Cathode

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Angewandte Chemie 2023年第25期135卷

作者： Zuoyu Qin Dr. Ying Zhang Wuqing Luo Tao Zhang Tao Wang Lianshan Ni Haoji Wang Prof. Ning Zhang Prof. Xiaohe Liu Jiang Zhou Prof. Gen Chen School of Materials Science and Engineering Hunan Provincial Key Laboratory of Electronic Packaging and Advanced Functional Materials Central South University 410083 Changsha Hunan P. R. China Contribution: Conceptualization (equal) Data curation (lead) Formal analysis (lead) Investigation (equal) Writing - original draft (lead) Zhongyuan Critical Metals Laboratory and School of Chemical Engineering Zhengzhou University 450001 Zhengzhou Henan P. R. China Contribution: Investigation (supporting) Visualization (lead) Writing - review & editing (equal) Contribution: Validation (lead) Contribution: Investigation (supporting) Resources (lead) Visualization (supporting) School of Metallurgy and Environment Central South University 410083 Changsha Hunan P. R. China Contribution: Investigation (supporting) Writing - review & editing (supporting) College of Chemistry and Chemical Engineering Central South University 410083 Changsha Hunan P. R. China Contribution: Formal analysis (supporting) Investigation (supporting) Contribution: Validation (supporting) Writing - review & editing (supporting) Contribution: Methodology (supporting) Writing - review & editing (supporting) Contribution: Project administration (supporting) Writing - review & editing (supporting) Contribution: Conceptualization (equal) Funding acquisition (equal) Investigation (lead) Project administration (supporting) Supervision (supporting) Writing - review & editing (lead) Contribution: Conceptualization (equal) Funding acquisition (lead) Investigation (equal) Project administration (lead) Supervision (lead)

With ever-increasing pursuit for high-value output in recycling spent lithium-ion batteries (LIBs), traditional recycling methods of cathodes tend to be obsolete because of the complicated procedures. Herein, we first upcycle spent polycrystal LiNi 0.88 Co 0.095 Al 0.025 O 2 (S-NCA) to high value-added single-crystalline and Li-rich cathode materials through a simple but feasible LiOH-Na 2 SO 4 eutectic molten salt strategy. The in situ X-ray diffraction technique and a series of paratactic experiments record the evolution process of upcycling and prove that excessive Li occupies the transition metal (TM) layers. Beneficial from the single-crystalline and Li-rich nature, the regenerated NCA (R-NCA) exhibits remarkably enhanced electrochemical performances in terms of long-term cyclability, high-rate performance and low polarization. This approach can also be successfully extended to other cathode materials e.g., LiNi x Co y Mn z O 2 (NCM) and mixed spent NCAs with varied degree of Li loss.

关键词： Li-Rich Cathode Single-Crystalline Spent LiNi0.88Co0.095Al0.025O2 Upcycling

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