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Reconstruction of Solid Electrolyte Interphase with SrI2Reactivates Dead Li for Durable Anode-Free Li-Metal Batteries

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Angewandte Chemie 2023年第23期135卷

作者： Dr. Liwei Dong Dr. Shijie Zhong Dr. Botao Yuan Dr. Yaqiang Li Dr. Jipeng Liu Dr. Yuanpeng Ji Dr. Dongjiang Chen Dr. Yuanpeng Liu Prof. Chunhui Yang Prof. Jiecai Han Prof. Weidong He National Key Laboratory of Science and Technology on Advanced Composites in Special Environments and Center for Composite Materials and Structures Harbin Institute of Technology Harbin 150080 China MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage School of Chemistry and Chemical Engineering Harbin Institute of Technology Harbin 150080 China State Key Laboratory of Urban Water Resource and Environment Harbin Institute of Technology Harbin 150080 China Contribution: Conceptualization (lead) Data curation (lead) Writing - original draft (lead) Contribution: Conceptualization (equal) Data curation (equal) Contribution: Data curation (equal) Investigation (equal) Contribution: Data curation (supporting) Writing - original draft (supporting) Contribution: Conceptualization (supporting) Data curation (supporting) Chongqing Research Institute Harbin Institute of Technology Chongqing 401151 China Contribution: Investigation (supporting) Writing - review & editing (supporting) Contribution: Data curation (supporting) Investigation (supporting) Contribution: Project administration (supporting) Resources (supporting) Contribution: Conceptualization (supporting) Project administration (supporting) Resources (supporting) School of Mechanical Engineering Chengdu University Chengdu 610106 China Contribution: Conceptualization (equal) Project administration (equal) Writing - original draft (equal)

Without excess Li, anode-free Li-metal batteries (AFLMBs) have been proposed as the most likely solution to realizing highly-safe and cost-effective Li-metal batteries. Nevertheless, short cyclic life puzzles conventional AFLMBs due to anodic dead Li accumulation with a local current concentration induced by irreversible electrolyte depletion, insufficient active Li reservoir and slow Li + transfer at the solid electrolyte interphase (SEI). Herein, SrI 2 is introduced into carbon paper (CP) current collector to effectively suppress dead Li through synergistic mechanisms including reversible I − /I 3 − redox reaction to reactivate dead Li, dielectric SEI surface with SrF 2 and LiF to prevent electrolyte decomposition and highly ionic conductive (3.488 mS cm −1 ) inner layer of SEI with abundant LiI to enable efficient Li + transfer inside. With the SrI 2 -modified current collector, the NCM532/CP cell delivers unprecedented cyclic performances with a capacity of 129.2 mAh g −1 after 200 cycles.

关键词： Anode-Free Li-Metal Batteries Current Collector Dead Li SrF2 SrI2

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Deploying Cationic Cellulose Nanofiber Confinement to Enable High Iodine Loadings Towards High Energy and High-Temperature Zn-I2Battery

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Angewandte Chemie 2023年第5期136卷

作者： Zhenglin Li Wenwen Cao Tao Hu Yichan Hu Rong Zhang Huilin Cui Funian Mo Chaozheng Liu Chunyi Zhi Guojin Liang Institute of Technology for Carbon Neutrality Shenzhen Institute of Advanced Technology Chinese Academy of Sciences (CAS) Shenzhen 518055 China Co-Innovation Center of Efficient Processing and Utilization of Forest Resources College of Materials Science and Engineering Nanjing Forestry University Nanjing 210000 China Contribution: Data curation (lead) Investigation (lead) Methodology (lead) Writing - original draft (lead) School of Chemistry and Chemical Engineering University of Jinan Jinan 250022 China Contribution: Conceptualization (equal) Data curation (lead) Investigation (lead) Methodology (lead) School of Materials Science and Engineering Key Laboratory of Structure and Functional Regulation of Hybrid Materials Ministry of Education Anhui University Hefei 230601 China Contribution: Data curation (equal) Formal analysis (equal) Investigation (supporting) Methodology (supporting) Contribution: Conceptualization (equal) Data curation (supporting) Formal analysis (equal) Investigation (equal) Department of Materials Science and Engineering City University of Hong Kong 83 Tat Chee Avenue Kowloon Hong Kong 999077 Hong Kong Contribution: Data curation (equal) Investigation (equal) Methodology (equal) Contribution: Conceptualization (supporting) Data curation (supporting) Formal analysis (equal) Investigation (equal) Shenzhen Key Laboratory of Flexible Printed Electronics Technology Center Harbin Institute of Technology Shenzhen Guangdong 518055 China Contribution: Conceptualization (lead) Data curation (lead) Resources (lead) Supervision (equal) Contribution: Conceptualization (equal) Data curation (lead) Investigation (lead) Supervision (equal) Contribution: Supervision (lead) Visualization (lead) Writing - review & editing (lead) Contribution: Conceptualization (lead) Supervision (lead) Writing - original draft (lead) Writing - review & editing (lead)

High iodine loading and high-temperature adaptability of the iodine cathode are prerequisites to achieving high energy density at full battery level and promoting the practical application for the zinc-iodine (Zn-I 2 ) battery. However, it would aggravate the polyiodide shuttle effect when employing high iodine loading and working temperature. Here, a sustainable cationic cellulose nanofiber (cCNF) was employed to confine the active iodine species through strong physiochemical adsorption to enlarge the iodine loading and stabilize it even at high temperatures. The cCNF could accommodate dual-functionality by enlarging the iodine loading and suppressing the polyiodide shuttle effect, owing to the unique framework structure with abundant surface positive charges. As a result, the iodine cathode based on the cCNF could deliver high iodine mass loading of 14.1 mg cm −2 with a specific capacity of 182.7 mAh g −1 , high areal capacity of 2.6 mAh cm −2 , and stable cycling over 3000 cycles at 2 A g −1 , thus enabling a high energy density of 34.8 Wh kg −1 and the maximum power density of 521.2 W kg −1 at a full Zn-I 2 battery level. In addition, even at a high temperature of 60 °C, the Zn-I 2 battery could still deliver a stable cycling.

关键词： Cationic Cellulose High- Temperature Battery Iodine Shuttle-Free Zn-I2 Battery

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Self-Assembled Monolayers of Bi-Functionalized Porphyrins: A Novel Class of Hole-Layer-Coordinating Perovskites and Indium Tin Oxide in Inverted Solar Cells

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Angewandte Chemie 2023年第40期135卷

作者： Chieh-Ming Hung Chi-Lun Mai Chi-Chi Wu Bo-Han Chen Chih-Hsuan Lu Che-Chun Chu Meng-Chuan Wang Prof. Shang-Da Yang Prof. Hsieh-Chih Chen Prof. Chen-Yu Yeh Prof. Pi-Tai Chou Department of Chemistry Center for Emerging Materials and Advanced Devices National Taiwan University 106319 Taipei Taiwan Contribution: Conceptualization (lead) Data curation (lead) Formal analysis (lead) Investigation (lead) Project administration (lead) Writing - original draft (lead) Department of Chemistry i-Center for Advanced Science and Technology (i-CAST) Innovation and Development Center of Sustainable Agriculture (IDCSA) National Chung Hsing University 402202 Taichung Taiwan Contribution: Data curation (supporting) Investigation (supporting) Project administration (equal) Resources (lead) Writing - original draft (lead) Contribution: Software (lead) Institute of Photonics Technologies National Tsing Hua University 300044 Hsinchu Taiwan Contribution: Data curation (lead) Formal analysis (lead) Contribution: Data curation (equal) Formal analysis (equal) Contribution: Data curation (supporting) Formal analysis (supporting) Investigation (supporting) Contribution: Data curation (supporting) Resources (supporting) Contribution: Writing - review & editing (supporting) Department of Chemistry Fu Jen Catholic University 242062 New Taipei City Taiwan Contribution: Writing - original draft (equal) Writing - review & editing (lead) Contribution: Writing - original draft (lead) Writing - review & editing (equal) Contribution: Writing - original draft (supporting) Writing - review & editing (lead)

Self-assembled monolayers (SAMs) offer the advantage of facile interfacial modification, leading to significant improvements in device performance. In this study, we report the design and synthesis of a new series of carboxylic acid-functionalized porphyrin derivatives, namely AC-1, AC-3, and AC-5, and present, for the first time, a strategy to exploit the large π-moiety of porphyrins as a backbone for interfacing the indium tin oxide (ITO) electrode and perovskite active layer in an inverted perovskite solar cell (PSC) configuration. The electron-rich nature of porphyrins facilitates hole transfer and the formation of SAMs, resulting in a dense surface that minimizes defects. Comprehensive spectroscopic and dynamic studies demonstrate that the double-anchored AC-3 and AC-5 enhance SAMs on ITO, passivate the perovskite layer, and function as conduits to facilitate hole transfer, thus significantly boosting the performance of PSCs. The champion inverted PSC employing AC-5 SAM achieves an impressive solar efficiency of 23.19 % with a high fill factor of 84.05 %. This work presents a novel molecular engineering strategy for functionalizing SAMs to tune the energy levels, molecular dipoles, packing orientations to achieve stable and efficient solar performance. Importantly, our comprehensive investigation has unraveled the associated mechanisms, offering valuable insights for future advancements in PSCs.

关键词： Functionalized Porphyrins Hole-Selective Layer Perovskite Solar Cells Self-Assembled Monolayers Transient Absorption Spectroscopy

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Iridium-Catalyzed Chemo-, Diastereo-, and Enantioselective Allyl-Allyl Coupling: Accessing All Four Stereoisomers of (E)-1-Boryl-Substituted 1,5-Dienes by Chirality Pairing

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Angewandte Chemie 2023年第13期135卷

作者： Yongsuk Jung Seok Yeol Yoo Yonghoon Jin Jaehyun You Seungcheol Han Jeongwoo Yu Prof. Dr. Yoonsu Park Prof. Dr. Seung Hwan Cho Department of Chemistry Pohang University of Science and Technology (POSTECH) Pohang 37673 (Republic of Korea Contribution: Conceptualization (supporting) Data curation (lead) Formal analysis (lead) Investigation (lead) Methodology (lead) Writing - original draft (supporting) Writing - review & editing (supporting) Department of Chemistry Korea Advanced Institute of Science and Technology (KAIST) Daejeon 34141 (Republic of Korea Contribution: Data curation (lead) Writing - original draft (supporting) Contribution: Data curation (supporting) Formal analysis (supporting) Contribution: Data curation (supporting) Contribution: Data curation (lead) Formal analysis (lead) Funding acquisition (lead) Writing - original draft (lead) Writing - review & editing (lead) Contribution: Conceptualization (lead) Formal analysis (lead) Funding acquisition (lead) Investigation (lead) Methodology (lead) Project administration (lead) Writing - original draft (lead) Writing - review & editing (lead)

Here, we report a highly chemo-, diastereo-, and enantioselective allyl-allyl coupling between branched allyl alcohols and α-silyl-substituted allylboronate esters, catalyzed by a chiral iridium complex. The α-silyl-substituted allylboronate esters can be chemoselectively coupled with allyl electrophiles, affording a diverse set of enantioenriched ( E )-1-boryl-substituted 1,5-dienes in good yields, with excellent stereoselectivity. By permuting the chiral iridium catalysts and the substrates, we efficiently and selectively obtained all four stereoisomers bearing two consecutive chiral centers. Mechanistic studies via density functional theory calculations revealed the origins of the diastereo- and chemoselectivities, indicating the pivotal roles of the steric interaction, the β-silicon effect, and a rapid desilylation process. Additional synthetic modifications for preparing a variety of enantioenriched compounds containing contiguous chiral centers are also included.

关键词： Allyl-Allyl Coupling Chemoselectivity Diastereoselectivity Enantioselectivity Stereoisomers

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Near-Stoichiometric and Homogenized Perovskite Films for Solar Cells with Minimized Performance Variation

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Angewandte Chemie 2023年第17期135卷

作者： Wenhuai Feng Junlei Tao Gengling Liu Guo Yang Dr. Jun-Xing Zhong Yuxuan Fang Li Gong Prof. Shaopeng Yang Prof. Wu-Qiang Wu Key Laboratory of Bioinorganic and Synthetic Chemistry (MoE) Lehn Institute of Functional Materials School of Chemistry Sun Yat-sen University Guangzhou 510006 China Contribution: Data curation (lead) Investigation (lead) Writing - original draft (lead) Province-Ministry Co-construction Collaborative Innovation Center of Hebei Photovoltaic Technology College of Physics Science and Technology Hebei University Baoding 071002 China Contribution: Data curation (equal) Formal analysis (equal) Contribution: Data curation (supporting) Formal analysis (supporting) Writing - original draft (supporting) Contribution: Data curation (supporting) Resources (supporting) Instrumental Analysis Research Center Sun Yat-sen University Guangzhou 510275 China Contribution: Data curation (supporting) Contribution: Conceptualization (lead) Funding acquisition (lead) Project administration (lead) Writing - original draft (lead) Writing - review & editing (lead)

Mixed-cation, small band-gap perovskites via rationally alloying formamidinium (FA) and methylammonium (MA) together have been widely employed for blade-coated perovskite solar cells with satisfied efficiencies. One of the stringent challenges lies in difficult control of the nucleation and crystallization kinetics of the perovskites with mixed ingredients. Herein, a pre-seeding strategy by mixing FAPbI 3 solution with pre-synthesized MAPbI 3 microcrystals has been developed to smartly decouple the nucleation and crystallization process. As a result, the time window of initialized crystallization has been greatly extended by 3 folds (i.e. from 5 s to 20 s), which enables the formation of uniform and homogeneous alloyed-FAMA perovskite films with designated stoichiometric ratios. The resultant blade-coated solar cells achieved a champion efficiency of 24.31 % accompanied by outstanding reproducibility with more than 87 % of the devices showing efficiencies higher than 23 %.

关键词： Blade-Coating Chemical Homogeneity Crystal Pre-Seeding Perovskite Solar Cells

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Mapping the Complete Photocycle that Powers a Large Stokes Shift Red Fluorescent Protein

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Angewandte Chemie 2022年第5期135卷

作者： Dr. Ziyu Wang Dr. Ya Zhang Dr. Cheng Chen Dr. Ruixue Zhu Dr. Jiaming Jiang Prof. Tsu-Chien Weng Prof. Quanjiang Ji Prof. Yifan Huang Prof. Chong Fang Prof. Weimin Liu School of Physical Science and Technology ShanghaiTech University 201210 Shanghai China Contribution: Data curation (equal) Formal analysis (lead) Investigation (equal) Methodology (equal) Resources (supporting) Visualization (lead) Writing - original draft (equal) Writing - review & editing (supporting) University of Chinese Academy of Sciences 100049 Beijing China Contribution: Data curation (supporting) Investigation (supporting) Methodology (equal) Resources (supporting) Writing - original draft (supporting) Department of Chemistry Oregon State University 153 Gilbert Hall 97331 Corvallis OR USA Contribution: Data curation (supporting) Formal analysis (supporting) Investigation (supporting) Validation (supporting) Visualization (supporting) Writing - review & editing (supporting) Contribution: Data curation (supporting) Investigation (supporting) Validation (supporting) Contribution: Investigation (supporting) Validation (supporting) Contribution: Data curation (supporting) Resources (supporting) Supervision (supporting) Validation (supporting) Contribution: Data curation (supporting) Resources (equal) Supervision (supporting) Validation (supporting) Contribution: Data curation (supporting) Funding acquisition (supporting) Resources (equal) Software (lead) Validation (supporting) Visualization (supporting) Contribution: Conceptualization (supporting) Data curation (supporting) Funding acquisition (equal) Investigation (supporting) Project administration (supporting) Resources (supporting) Supervision (supporting) Validation (supporting) Visualization (equal) Writing - review & editing (lead) Contribution: Conceptualization (lead) Data curation (equal) Funding acquisition (lead) Investigation (supporting) Methodology (lead) Project administration (lead) Resources (equal) Supervision (lead) Validation (supporting) Writing - original draft (equal) Writing - review & editing (supporting)

Large Stokes shift (LSS) red fluorescent proteins (RFPs) are highly desirable for bioimaging advances. The RFP mKeima, with coexisting cis- and trans -isomers, holds significance as an archetypal system for LSS emission due to excited-state proton transfer (ESPT), yet the mechanisms remain elusive. We implemented femtosecond stimulated Raman spectroscopy (FSRS) and various time-resolved electronic spectroscopies, aided by quantum calculations, to dissect the cis - and trans -mKeima photocycle from ESPT, isomerization, to ground-state proton transfer in solution. This work manifests the power of FSRS with global analysis to resolve Raman fingerprints of intermediate states. Importantly, the deprotonated trans -isomer governs LSS emission at 620 nm, while the deprotonated cis -isomer's 520 nm emission is weak due to an ultrafast cis -to- trans isomerization. Complementary spectroscopic techniques as a table-top toolset are thus essential to study photochemistry in physiological environments.

关键词： Chromophore Isomerization Excited- and Ground-State Proton Transfer Femtosecond Raman Spectroscopy Large Stokes Shift Red Fluorescent Proteins

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Noninvasive genetic monitoring of Chinese pangolin (Manis pentadactyla) from Darjeeling district of Northwest Bengal, India

Wildlife Letters

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Wildlife Letters 2023年第1期1卷

作者： Prajnashree Priyambada Vinaya K. Singh Abhishek Singh Bheem D. Joshi Supriyo Dalui Lenrik K. Wangmo Avijit Ghosh Avantika Thapa Sujeet K. Singh Kailash Chandra Lalit K. Sharma Mukesh Thakur Mammal and Osteology Section Zoological Survey of India New Alipore Kolkata West Bengal India Department of Zoology University of Calcutta Kolkata West Bengal India Contribution: Conceptualization (equal) Data curation (equal) Methodology (equal) Writing - original draft (equal) Contribution: Conceptualization (equal) Data curation (equal) Methodology (equal) Writing - original draft (equal) Writing - review & editing (equal) Contribution: Conceptualization (equal) Data curation (equal) Validation (equal) Writing - original draft (equal) Contribution: Conceptualization (equal) Methodology (equal) Supervision (equal) Writing - original draft (equal) Writing - review & editing (equal) Contribution: Data curation (equal) Methodology (equal) Visualization (equal) Writing - review & editing (equal) Contribution: Formal analysis (equal) Software (supporting) Contribution: Formal analysis (supporting) Software (equal) Contribution: Data curation (equal) Contribution: Conceptualization (equal) Supervision (equal) Writing - review & editing (equal) Contribution: Project administration (equal) Supervision (equal) Contribution: Investigation (equal) Project administration (equal) Supervision (equal) Writing - review & editing (equal)

Chinese pangolin ( Manis pentadactyla ) has experienced a rapid population decline across its distribution range mainly due to illegal harvesting for scale and local consumption for meat. We monitored 65 burrows of free-ranging pangolins and collected 147 fecal droppings from five sites in the Darjeeling district of Northwest Bengal in the central Himalayas. On genetic analysis with the mitochondrial cytochrome b gene, we obtained four haplotypes with haplotype diversity of 0.479 ± 0.088. At 15 microsatellite loci, we identified 35 unique genotypes with relatively low level of genetic diversity (Ho-0.382 ± 0.091). We also estimated the population genetic parameters and demographic history using Bayesian skyline plot which revealed a demographic decline in the population size in the past 200 years. The present study generated the base-line population genetics estimates of Chinese pangolin, that may be used in genetic monitoring of the population and also aid to the geographical assignment of wildlife crime cases. 中华穿山甲（Manis pentadactyla）种群数量在其分布区内迅速下降，主要是因为非法利用其甲片以及当地食用其肉。在喜马拉雅山脉中部印度西孟加拉邦的大吉岭地区的5个地点，我们监测了65个中华穿山甲的野外洞穴，并收集了147份粪便样品。基于线粒体细胞色素b（Cytb）基因片段的遗传分析，获得4个单倍型，其单倍型多样性为0.479±0.088。应用15个微卫星位点的遗传进行分析，鉴定出35个遗传多样性相对较低的基因型（观测杂合度为0.382±0.091）。使用贝叶斯天际线模型（Bayesian skyline plot,BSP），估算了种群遗传参数与历史动态，发现200年前中华穿山甲的种群规模就已经开始出现明显下降。本研究提供了中华穿山甲种群遗传评估的基准状况，可用于中华穿山甲种群遗传监测和非法制品地理来源鉴定。 Researchers/biologists can utilize the baseline population genetic estimates in this paper to undertake comparisons in evaluating genetic diversity patterns among different regions with respect to anthropogenic activities and land use. The genotype data generated may be utilized by researchers/biologists in evaluating the population size of Chinese pangolin following the capture–recapture framework. The regional genetic signature generated in this study may be used by the wildlife forensic professionals/scientists in assigning the wildlife contraband to the source of origin.

关键词： conservation genetics Cyt b Darjeeling Manis pentadactyla microsatellite 保护遗传学细胞色素b 大吉岭中华穿山甲微卫星

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Intrinsic Phase Stability and Inherent Bandgap of Formamidinium Lead Triiodide Perovskite Single Crystals

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Angewandte Chemie 2022年第50期134卷

作者： Dr. Liang Chen Jin Wook Yoo Manman Hu Seung-Un Lee Prof. Sang Il Seok Department of Energy and Chemical Engineering Ulsan National Institute of Science and Technology 50 UNIST-gil Eonyang-eup Ulju-gun Ulsan 44919 Republic of Korea Contribution: Conceptualization (equal) Data curation (lead) Investigation (lead) Writing - original draft (equal) Contribution: Data curation (supporting) Formal analysis (supporting) Contribution: Investigation (supporting) Methodology (supporting) Contribution: Formal analysis (supporting) Contribution: Supervision (lead) Writing - review & editing (supporting)

Understanding the intrinsic phase stability and inherent band gap of formamidinium lead triiodide (FAPbI 3 ) perovskites is crucial to further improve the performance of perovskite solar cells (PSCs). Herein, we explored the α- to δ-phase transition and band gap of FAPbI 3 single crystals grown by an inverse temperature solubility method. We found that the residual γ-butyrolactone solvents in the inner empty space of the FAPbI 3 single crystal accelerate the phase transition at kinetics. By adopting 2-methoxyethanol as the solvent, over 2000 h of stable α-FAPbI 3 crystals could be acquired. This proves that although FAPbI 3 is regarded as unstable at thermodynamics, it could own excellent kinetic stability without any doping or additives because of the slow solid to solid phase transition instead of the fast phase transition assisted by the solvents. Furthermore, we revealed that the bulk FAPbI 3 single crystal with a size above 100 μm can have an inherent band gap of 1.41 eV. Thus, our work provides key scientific guidance for high-performance FAPbI 3 -based PSCs.

关键词： FAPbI3 Inherent Band Gap Intrinsic Phase Stability Perovskite Single Crystal

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Cover Image, Volume 9, Issue 2

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WIREs Water 2022年第2期9卷

作者： Zeqing Huang Tongtiegang Zhao Contribution: Data curation (equal) Formal analysis (equal) Visualization (equal) Contribution: Conceptualization (equal) Formal analysis (equal) Funding acquisition (lead) Resources (equal) Supervision (lead)

The cover image is based on the Advanced Review Predictive performance of ensemble hydroclimatic forecasts: Verifi cation metrics, diagnostic plots and forecast attributes by Zeqing Huang and Tongtiegang Zhao https://...

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Cover Image, Volume 139, Issue 45

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Journal of Applied Polymer Science 2022年第45期139卷

作者： Satoshi Horikoshi Yuhei Arai Haruka Mura Nick Serpone Contribution: Conceptualization (lead) Funding acquisition (lead) Methodology (lead) Supervision (lead) Writing - original draft (lead) Contribution: Data curation (lead) Formal analysis (lead) Contribution: Formal analysis (lead) Contribution: Writing - review & editing (lead)

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