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Discovering the Intrinsic Causes of Dendrite Formation in Zinc Metal Anodes: Lattice Defects and Residual Stress

Angewandte Chemie 2023年第16期135卷

作者： Chunlin Xie Shengfang Liu Zefang Yang Huimin Ji Shuhan Zhou Hao Wu Chao Hu Yougen Tang Xiaobo Ji Qi Zhang Haiyan Wang Hunan Provincial Key Laboratory of Chemical Power Sources College of Chemistry and Chemical Engineering Central South University Changsha 410083 P. R. China Contribution: Conceptualization (lead) Data curation (lead) Formal analysis (lead) Investigation (lead) Visualization (lead) Writing - original draft (lead) College of Chemistry and Chemical Engineering Northwest Normal University Lanzhou 730070 China Contribution: Conceptualization (equal) Data curation (equal) Formal analysis (equal) Contribution: Validation (equal) Visualization (equal) Contribution: Investigation (equal) Methodology (equal) Contribution: Investigation (equal) Contribution: Project administration (equal) Resources (equal) Contribution: Conceptualization (equal) Data curation (equal) Resources (equal)

Developing a highly stable and dendrite-free zinc anode is essential to the commercial application of zinc metal batteries. However, the understanding of zinc dendrites formation mechanism is still insufficient. Herein, for the first time, we discover that the interfacial heterogeneous deposition induced by lattice defects and epitaxial growth limited by residual stress are intrinsic and critical causes for zinc dendrite formation. Therefore, an annealing reconstruction strategy was proposed to eliminate lattice defects and stresses in zinc crystals, which achieve dense epitaxial electrodeposition of zinc anode. The as-prepared annealed zinc anodes exhibit dendrite-free morphology and enhanced electrochemical cycling stability. This work first proves that lattice defects and residual stresses are also very important factors for epitaxial electrodeposition of zinc in addition to crystal orientation, which can provide a new mechanism for future researches on zinc anode modification.

关键词： Crystal Defects Dendrite Epitaxial Growth Residual Stress Zinc Anode

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Generation of Tunable Ultrastrong White-Light Emission by Activation of a Solid Supramolecule through Bromonaphthylpyridinium Polymerization

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Angewandte Chemie 2022年第44期134卷

作者： Dr. Yu-Yang Hu Xian-Yin Dai Xiaoyun Dong Man Huo Prof. Dr. Yu Liu College of Chemistry State Key Laboratory of Elemento-Organic Chemistry Nankai University Tianjin 300071 P. R. China Contribution: Data curation (equal) Formal analysis (equal) Investigation (equal) Methodology (equal) Validation (equal) Writing - original draft (equal) Contribution: Data curation (equal) Formal analysis (equal) Investigation (equal) Validation (equal) Writing - original draft (equal) Contribution: Data curation (supporting) Investigation (supporting) Methodology (supporting) Validation (supporting) Contribution: Investigation (supporting) Methodology (supporting) Validation (supporting)

Herein, we reported solid supramolecular bromonaphthylpyridinium polymers (P-BrNp), which exhibit tunable phosphorescence emission in the amorphous state enabled by sulfobutylether-β-cyclodextrin (SBE-β-CD) and diarylethene derivatives. The monomer BrNp gave single fluorescence emission at 490 nm, while an apparent room-temperature phosphorescence (RTP) at 550 nm emerged for P-BrNp copolymers with various feed ratios. Through fluorescence-phosphorescence dual emission, P-BrNp-0.1 displayed an ultrahigh white-light emission quantum yield of 83.9 %. Moreover, the subsequent assembly with SBE-β-CD further enhanced the phosphorescent quantum yield of P-BrNp-0.1 from 64.1 % to 71.3 %, accompanied by the conversion of photoluminescence emission from white to yellow. Diarylethene monomers were introduced as photoswitches to realize reversible RTP emission, which can be used in switchable data encryption and multifunctional writing ink.

关键词： Bromonaphthylpyridinium Phosphorescence Polymerization Sulfobutylether-β-Cyclodextrin White-Light Emission

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Polymeric Carbon Nitride with Chirality Inherited from Supramolecular Assemblies

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Angewandte Chemie 2023年第40期135卷

作者： Adi Azoulay Sapir Shekef Aloni Prof. Lidan Xing Ayelet Tashakory Prof. Yitzhak Mastai Prof. Menny Shalom Department of Chemistry and Ilse Katz Institute for Nanoscale Science and Technology Ben-Gurion University of the Negev Beer-Sheva 8410501 Israel Contribution: Conceptualization (lead) Data curation (lead) Formal analysis (lead) Writing - original draft (lead) Department of Chemistry and Institute of Nanotechnology and Advanced Materials Bar-Ilan University Ramat-Gan 5290002 Israel Contribution: Conceptualization (equal) Data curation (equal) Formal analysis (equal) Writing - original draft (equal) School of Chemistry South China Normal University Guangzhou 510006 China Contribution: Data curation (supporting) Formal analysis (supporting) Methodology (supporting) Software (supporting) Writing - review & editing (supporting) Contribution: Data curation (supporting) Formal analysis (supporting) Investigation (supporting) Writing - review & editing (supporting) Contribution: Conceptualization (equal) Data curation (supporting) Project administration (equal) Resources (equal) Supervision (equal) Writing - review & editing (equal) Contribution: Conceptualization (lead) Data curation (equal) Funding acquisition (lead) Project administration (lead) Supervision (lead) Writing - review & editing (lead)

The facile synthesis of chiral materials is of paramount importance for various applications. Supramolecular preorganization of monomers for thermal polymerization has been proven as an effective tool to synthesize carbon and carbon nitride-based (CN) materials with ordered morphology and controlled properties. However, the transfer of an intrinsic chemical property, such as chirality from supramolecular assemblies to the final material after thermal condensation, was not shown. Here, we report the large-scale synthesis of chiral CN materials capable of enantioselective recognition. To achieve this, we designed supramolecular assemblies with a chiral center that remains intact at elevated temperatures. The optimized chiral CN demonstrates an enantiomeric preference of ca. 14 %; CN electrodes were also prepared and show stereoselective interactions with enantiomeric probes in electrochemical measurements. By adding chirality to the properties transferrable from monomers to the final product of a thermal polymerization, this study confirms the potential of using supramolecular precursors to produce carbon and CN materials and electrodes with designed chemical properties.

关键词： Carbon Nitride Chiral Recognition Chirality Enantioselective Material Supramolecular Assembly

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Crystallization Regulation by Self-Assembling Liquid Crystal Template Enables Efficient and Stable Perovskite Solar Cells

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Angewandte Chemie 2023年第52期135卷

作者： Meizi Wu Hongyan Wang Yong Li Dr. Ran Chen Hui Zhou Shaomin Yang Dongfang Xu Kun Li Prof. Dr. Zhongwei An Shengzhong (Frank) Liu Prof. Dr. Zhike Liu Key Laboratory of Applied Surface and Colloid Chemistry Ministry of Education Shaanxi Key Laboratory for Advanced Energy Devices Shaanxi Engineering Lab for Advanced Energy Technology International Joint Research Center of Shaanxi Province for Photoelectric Materials Science School of Materials Science & Engineering Shaanxi Normal University Xi'an 710119 P. R. China Contribution: Data curation (lead) Formal analysis (lead) Investigation (lead) Writing - original draft (lead) Contribution: Data curation (equal) Formal analysis (equal) Contribution: Data curation (equal) Investigation (equal) School of Materials Science and Engineering Xi' an University of Science and Technology Xi'an 710054 P. R. China Contribution: Conceptualization (lead) Methodology (equal) Contribution: Formal analysis (equal) Investigation (equal) Contribution: Methodology (equal) Contribution: Data curation (equal) Contribution: Investigation (equal) Contribution: Conceptualization (equal) Methodology (equal) Contribution: Conceptualization (equal) Methodology (equal) Writing - review & editing (lead)

It is found that the disordered growth of bottom perovskite film deteriorates the buried interface of perovskite solar cells (PSCs), so developing a new material to modify the buried interface for regulating the crystal growth and defect passivation is an effective approach for improving the photovoltaic performance of PSCs. Here, we developed a new ionic liquid crystal (ILC, 1-Dodecyl-3-methylimidazolium tetrafluoroborate) as both crystal regulator and defect passivator to modify the buried interface of PSCs. The high lattice matching between this ILC and perovskite promotes preferential growth of perovskite film along [001] direction, while the oriented ILC with mesomorphic phase has a strong chemical interaction with perovskite to passivate the interface defect, as a result, the modified buried interface exhibits suppressed defects, improved band alignment, reduced nonradiative recombination losses, and enhanced charge extraction. The ILC-modified PSC delivers a power conversion efficiency of 24.92 % and maintains 94 % of the original value after storage in ambient for 3000 h.

关键词： Crystallization Regulation Ionic Liquid Crystals Perovskite Solar Cells Self-Assembling

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Evolution of a Strategy for Concise Enantioselective Total Synthesis of the Salinosporamide Family of Natural Products

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Angewandte Chemie 2022年第41期134卷

作者： Soojun Park Jiwoo Lee Prof. Dr. Jae Hyun Kim Yeji Jeong Dr. Seokwoo Lee Su Won Lee Prof. Dr. Sanghee Kim College of Pharmacy Seoul National University 1 Gwanak-ro Gwanak-gu Seoul 08826 Republic of Korea Contribution: Conceptualization (lead) Formal analysis (lead) Investigation (lead) Software (lead) Visualization (lead) Writing - original draft (lead) Contribution: Data curation (supporting) Formal analysis (supporting) Validation (supporting) Writing - original draft (supporting) College of Pharmacy Chung-Ang University 84 Heukseok-ro Seoul 06974 Republic of Korea Contribution: Conceptualization (equal) Formal analysis (equal) Project administration (supporting) Contribution: Data curation (supporting) Writing - original draft (supporting) Contribution: Visualization (supporting) Contribution: Data curation (supporting) Contribution: Conceptualization (lead) Project administration (lead) Supervision (lead) Writing - review & editing (lead)

Our first strategy for rapidly accessing pyrrolidinone cores of salinosporamides involved combined use of memory of chirality and dynamic kinetic resolution principles in aldol reactions of the serine-derived 5-oxazolidinone substrate, which was ultimately unsuccessful with respect to enantioselectivity. This failure led us to the revised strategy. The influence of the stereocenter in 5-oxazolidinone enabled selective installation of the C-2 stereocenter. The intramolecular aldol reaction of the C-2 stereodefined aldol substrate was successful. An unexpected hydrolytic dynamic kinetic resolution was observed in hydrolyses of the bicyclic aldol products. This unprecedented substrate-driven hydrolytic dynamic kinetic resolution was utilized in preparing the pyrrolidinone core with excellent efficiency. Through this strategy, the concise total syntheses of salinosporamides A and B as well as cinnabaramides A, E, and F were achieved with high selectivity.

关键词： Heterocycles Kinetic Resolution Natural Products Salinosporamides Total Synthesis

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Confinement-Driven Photophysics in Hydrazone-Based Hierarchical Materials

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Angewandte Chemie 2022年第2期135卷

作者： Grace C. Thaggard Dr. Gabrielle A. Leith Daniil Sosnin Dr. Corey R. Martin Kyoung Chul Park Margaret K. McBride Dr. Jaewoong Lim Brandon J. Yarbrough Buddhima K. P. Maldeni Kankanamalage Gina R. Wilson Austin R. Hill Dr. Mark D. Smith Prof. Dr. Sophya Garashchuk Prof. Dr. Andrew B. Greytak Prof. Dr. Ivan Aprahamian Prof. Dr. Natalia B. Shustova Department of Chemistry and Biochemistry University of South Carolina Columbia SC 29208 USA Contribution: Data curation (lead) Formal analysis (lead) Investigation (lead) Methodology (lead) Visualization (lead) Writing - original draft (lead) Writing - review & editing (supporting) Department of Chemistry Dartmouth College Hanover NH 03755 USA Contribution: Formal analysis (supporting) Investigation (lead) Visualization (supporting) Savannah River National Laboratory Aiken SC 29808 USA Contribution: Investigation (supporting) Methodology (lead) Writing - review & editing (supporting) Contribution: Formal analysis (supporting) Investigation (supporting) Methodology (lead) Writing - review & editing (supporting) Contribution: Data curation (supporting) Investigation (supporting) Contribution: Data curation (supporting) Writing - review & editing (supporting) Contribution: Data curation (supporting) Investigation (supporting) Writing - review & editing (supporting) Contribution: Data curation (supporting) Formal analysis (supporting) Investigation (supporting) Contribution: Data curation (supporting) Formal analysis (supporting) Contribution: Formal analysis (supporting) Funding acquisition (supporting) Resources (supporting) Software (lead) Supervision (supporting) Writing - original draft (supporting) Writing - review & editing (supporting) Contribution: Formal analysis (supporting) Visualization (supporting) Writing - review & editing (supporting) Contribution: Formal analysis (supporting) Resources (supporting) Supervision (supporting) Visualization (lead) Writing - review & editing (supporting)

Confinement-imposed photophysics was probed for novel stimuli-responsive hydrazone-based compounds demonstrating a conceptual difference in their behavior within 2D versus 3D porous matrices for the first time. The challenges associated with photoswitch isomerization arising from host interactions with photochromic compounds in 2D scaffolds could be overcome in 3D materials. Solution-like photoisomerization rate constants were realized for sterically demanding hydrazone derivatives in the solid state through their coordinative immobilization in 3D scaffolds. According to steady-state and time-resolved photophysical measurements and theoretical modeling, this approach provides access to hydrazone-based materials with fast photoisomerization kinetics in the solid state. Fast isomerization of integrated hydrazone derivatives allows for probing and tailoring resonance energy transfer (ET) processes as a function of excitation wavelength, providing a novel pathway for ET modulation.

关键词： Covalent-Organic Frameworks FRET Hydrazone Metal-Organic Frameworks Photochromism

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Organic Zinc-Ion Battery: Planar, π-Conjugated Quinone-Based Polymer Endows Ultrafast Ion Diffusion Kinetics

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Angewandte Chemie 2022年第51期134卷

作者： Dr. Fei Ye Qiang Liu Dr. Hongliang Dong Kailin Guan Zhaoyang Chen Na Ju Prof. Linfeng Hu School of Materials Science and Engineering Southeast University Nanjing 211189 China Contribution: Conceptualization (supporting) Data curation (lead) Investigation (lead) Writing - original draft (lead) Contribution: Data curation (equal) Formal analysis (equal) Software (lead) Center for High Pressure Science and Technology Advanced Research Shanghai 201203 P. R. China Contribution: Investigation (equal) Methodology (equal) Resources (equal) Validation (lead) Contribution: Formal analysis (equal) Investigation (lead) Methodology (equal) Contribution: Investigation (equal) Software (equal) Validation (lead) Visualization (lead) Contribution: Data curation (equal) Formal analysis (equal) Writing - original draft (supporting) Contribution: Conceptualization (lead) Data curation (lead) Formal analysis (lead) Funding acquisition (lead) Project administration (lead) Supervision (lead) Writing - original draft (lead) Writing - review & editing (lead)

A novel poly(phenazine-alt-pyromellitic anhydride) (PPPA) has been successfully designed and synthesized via a condensation polymerization strategy as promising cathode material in organic zinc-ion batteries. Electrochemical quartz crystal microbalance (EQCM), FTIR and XPS characterizations verify a reversible Zn 2+ -coordination mechanism in our PPPA cathode. Intriguingly, an ultrahigh Zn 2+ diffusion coefficient of 1.2×10 −7 cm 2 s −1 was found in this large π-conjugated system, which is the highest one among all organic cathode materials for zinc-ion batteries. Theoretical calculations reveal the extended π-conjugated plane in our PPPA sample results in a significant reduction on energy gap, effectively accelerating intramolecular electron transfer during charge/discharge process. Our finding provides insights to achieve high zinc-ion transport kinetics by a design strategy on planar polymer system.

关键词： Energy Gap Linear Polymer Organic Zinc-Ion Batteries Quinone-Based Polymer Zn2+ Diffusion Coefficient

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Cover Image, Volume 12, Issue 4

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WIREs Computational Molecular Science 2022年第4期12卷

作者： Duan Ni Zongtao Chai Ying Wang Mingyu Li Zhengtian Yu Yaqin Liu Shaoyong Lu Jian Zhang Contribution: Conceptualization (equal) Data curation (equal) Formal analysis (equal) Writing - original draft (lead) Writing - review & editing (equal) Contribution: Conceptualization (equal) Data curation (equal) Formal analysis (equal) Writing - review & editing (equal) Contribution: Data curation (equal) Formal analysis (equal) Contribution: Conceptualization (equal) Formal analysis (equal) Writing - review & editing (equal) Contribution: Formal analysis (equal) Resources (equal) Supervision (equal) Writing - review & editing (equal) Contribution: Conceptualization (lead) Formal analysis (equal) Funding acquisition (lead) Resources (equal) Supervision (lead) Writing - review & editing (lead) Contribution: Conceptualization (lead) Formal analysis (equal) Funding acquisition (lead) Resources (equal) Supervision (lead) Writing - review & editing (equal)

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Cover Image, Volume 140, Issue 25

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Journal of Applied Polymer Science 2023年第25期140卷

作者： Chia-Hui Chao Wei-Chuan Chen Chung-Yu Kuo Chun-Yen Liu Contribution: Data curation (lead) Formal analysis (lead) Investigation (lead) Methodology (supporting) Software (supporting) Contribution: Formal analysis (supporting) Methodology (supporting) Software (supporting) Visualization (equal) Contribution: Data curation (supporting) Formal analysis (supporting) Software (supporting) Visualization (supporting) Contribution: Conceptualization (lead) Funding acquisition (lead) Project administration (lead) Supervision (lead) Writing - original draft (lead) Writing - review & editing (lead)

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Pyrrolidone ligand improved Cu-based catalysts with high performance for acetylene hydrochlorination

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Applied Organometallic Chemistry 2020年第1期35卷

作者： You Han Yulian Wang Yan Wang Yubing Hu Yao Nian Wei Li Jinli Zhang School of Chemical Engineering and Technology Tianjin University Tianjin 300072 China Contribution: Conceptualization Formal analysis Funding acquisition Project administration Supervision Contribution: Conceptualization Data curation Investigation Methodology Contribution: Investigation Contribution: Validation Contribution: Visualization Contribution: Resources School of Chemistry and Chemical Engineering Shihezi University Shihezi 832003 China Contribution: Resources Supervision

A series of Cu-pyrrolidone/spherical activated carbon (SAC) catalysts were prepared via a simple incipient wetness impregnation method and then assessed in acetylene hydrochlorination, and the catalytic evaluation result indicated that the 1-methyl-2-pyrrolidinone (NMP) ligand was found to be the most effective one to significantly improve the activity and stability of Cu catalyst. The catalyst with the optimal molar ratio of NMP/Cu = 0.25 showed 94.2% acetylene conversion at 180°C and an acetylene gas hourly space velocity of 180 h −1 . Moreover, the acetylene conversion of Cu-0.25NMP/SAC remained stable over 99.1% for about 220 h under the industrial condition. Transmission electron microscopy (TEM) analyses proved that NMP ligand improved the dispersion of Cu species. In addition, hydrogen temperature-programmed reduction (H 2 -TPR), X-ray photoelectron spectra (XPS), thermogravimetric analysis (TGA), and Brunner–Emmet–Teller (BET) indicated that the additive of NMP was preferential to stabilize the catalytic active Cu + and Cu 2+ species and inhibit the reduction of Cu α+ to Cu 0 during the preparation process and reaction, hence restraining the coke deposition. Furthermore, the steady coordination structure between Cu and NMP was confirmed by Fourier-transform infrared spectra (FT-IR) and Raman combining with density functional theory (DFT) calculation, which could effectively lower the adsorption energy of catalyst for C 2 H 2 and inhibit the serious carbon deposition caused by excessive acetylene self-accumulation. Our findings suggest that the efficient, well-stabilized cost-effective, and environmentally friendly Cu catalyst has great potential in acetylene hydrochlorination.

关键词： acetylene hydrochlorination catalytic activity coordination Cu-based catalyst pyrrolidone ligand

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