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Computer-Aided Discovery of Potent Broad-Spectrum Vaccine Adjuvants

Angewandte Chemie 2023年第18期135卷

作者： Juan Ma Shenqing Wang Chuanfang Zhao Xiliang Yan Quanzhong Ren Zheng Dong Jiahuang Qiu Yin Liu Qing'e Shan Ming Xu Bing Yan Sijin Liu State Key Laboratory of Environmental Chemistry and Ecotoxicology Research Center for Eco-Environmental Sciences Chinese Academy of Sciences Beijing 100085 P. R. China School of Environmental Sciences University of Chinese Academy of Sciences Beijing 100049 P. R. China Contribution: Data curation (lead) Formal analysis (lead) Funding acquisition (supporting) Investigation (lead) Methodology (equal) Visualization (equal) Writing - original draft (lead) Institute of Environmental Research at Greater Bays Key Laboratory for Water Quality and Conservation of the Pearl River Delta Ministry of Education Guangzhou University Guangzhou 510006 P. R. China Contribution: Conceptualization (equal) Data curation (equal) Formal analysis (supporting) Investigation (supporting) Methodology (lead) School of Chemical Sciences University of Chinese Academy of Sciences Beijing 100049 P. R. China Contribution: Methodology (supporting) Software (lead) Visualization (lead) Contribution: Methodology (supporting) Software (lead) Visualization (supporting) Department of toxicology and sanitary chemistry School of public health Capital Medical University Beijing 100069 P. R. China Contribution: Data curation (supporting) Investigation (supporting) School of Environment Hangzhou Institute for Advanced Study University of Chinese Academy of Sciences Hangzhou 330106 P. R. China Contribution: Formal analysis (supporting) Methodology (supporting) Medical Science and Technology Innovation Center Shandong First Medical University & Shandong Academy of Medical Sciences Jinan Shandong 250117 P. R. China Contribution: Investigation (supporting) Contribution: Supervision (supporting) Contribution: Conceptualization (equal) Funding acquisition (supporting) Methodology (supporting) Project administration (equal) Writing - review & editing (equal) Contribution: Conceptualization (equal) Funding acquisition (lead) Project administration (lead) Supervision (lead) Writing - review & editing (lead)

Adjuvants stimulate the immune system to vigorously respond to a vaccine. While current adjuvants such as aluminum salts and oil-in-water emulsions have been used for decades, they do not generate broad and long-lasting responses in many vaccines. Consequently, more potent adjuvants are needed. Here, using computer-aided molecule design and machine learning, we discovered 2 new, broad-spectrum adjuvants that can boost vaccine responses. Our library containing 46 toll-like receptor (TLR)-targeting agonist ligands were assembled on Au nanoparticles. Comprehensive in vitro , ex vivo and in vivo studies showed both leads promoted dendritic cell activation via multiple TLRs and enhanced antigen presentation to T cells. When used together with tumor-specific antigens to immunize mice against B16-OVA melanoma and 4T1-PD1 breast cancer, both adjuvants unleashed strong immune responses that suppressed tumor growth and lung metastases. Our results show computer-aided design and screening can rapidly uncover potent adjuvants for tackling waning immunity in current vaccines.

关键词： Cancer Immunotherapy Computer-Aided Design Dendritic Cell Nano Adjuvant Pattern Recognition Receptor

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In Situ Reprogramming of Tumor-Associated Macrophages with Internally and Externally Engineered Exosomes

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Angewandte Chemie 2023年第11期135卷

作者： Dr. Lingmin Zhang Yinshan Lin Dr. Songpei Li Xiaoling Guan Xingyu Jiang Shenzhen Key Laboratory of Smart Healthcare Engineering Guangdong Provincial Key Laboratory of Advanced Biomaterials Department of Biomedical Engineering Southern University of Science and Technology No. 1088 Xueyuan Rd Nanshan District 518055 Shenzhen Guangdong China Guangzhou Municipal and Guangdong Provincial Key Laboratory of Molecular Target & Clinical Pharmacology the NMPA and State Key Laboratory of Respiratory Disease School of Pharmaceutical Sciences and the Fifth Affiliated Hospital Guangzhou Medical University 511436 Guangzhou Guangdong China Contribution: Conceptualization (lead) Formal analysis (equal) Funding acquisition (equal) Project administration (equal) Supervision (equal) Writing - review & editing (lead) Contribution: Data curation (lead) Formal analysis (lead) Methodology (lead) Software (lead) Validation (lead) Visualization (lead) Contribution: Investigation (equal) Methodology (equal) Software (equal) Writing - original draft (lead) Contribution: Investigation (supporting) Methodology (supporting) Software (supporting) Validation (supporting) Contribution: Conceptualization (equal) Funding acquisition (lead) Project administration (lead) Resources (lead) Supervision (lead)

The reprogramming of tumor-associated macrophages (TAMs) has emerged as an efficient strategy for immunotherapy. However, most of the approaches did not allow the in situ reprogramming of TAM because their low efficiency, non-specificity, or potential side effects. Herein, we produced exosomes with the clustered regularly interspaced short palindromic repeats interference (CRISPRi) internally engineered and the TAM specific peptide externally engineered onto the exosome membrane. The i nternally and e xternally e ngineered e xosomes ( IEEE , also named as I3E ) allowed the selective homing to tumor tissue and targeted to M2-like TAMs, which nearly repressed the expression of PI-3 kinase gamma (PI3Kγ) completely, and induced the TAMs polarizing to M1 both in vitro and in vivo. The polarized M1 macrophages awakened the “hot” tumor-immunity, causing the increase of T lymphocyte infiltration and the decrease of myeloid-derived suppressor cells, and inhibiting the tumor growth significantly. I3E reprogramed TAMs in situ precisely and efficiently.

关键词： CRISPRi Engineered Exosomes In Situ Reprogramming Lung Cancer Tumor-Associated Macrophages

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Modulating Ligand-Exchange Dynamics on Metal-Organic Polyhedra for Reversible Sorting and Hybridization of Miktoarm Star Polymers

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Angewandte Chemie 2023年第49期135卷

作者： Yuyan Lai Xiaofeng He Binghui Xue Mu Li Dr. Huihui Wang Dr. Wei Huang Dr. Jia-Fu Yin Dr. Mingxin Zhang Prof. Dr. Panchao Yin State Key Laboratory of Luminescent Materials and Devices South China Advanced Institute for Soft Matter Science and Technology South China University of Technology Guangzhou 510640 P. R. China Contribution: Investigation (lead) Methodology (equal) Writing - original draft (equal) Contribution: Investigation (equal) Methodology (supporting) Writing - original draft (equal) Contribution: Data curation (equal) Methodology (supporting) Validation (supporting) Contribution: Formal analysis (equal) Resources (supporting) Validation (supporting) State Key Laboratory of Marine Resource Utilization in South China Sea Hainan Provincial Key Lab of Fine Chemistry School of Chemical Engineering and Technology Hainan University Haikou Hainan 570228 P. R. China Contribution: Methodology (supporting) Validation (supporting) Contribution: Formal analysis (supporting) Validation (supporting) Contribution: Formal analysis (supporting) Visualization (supporting) Contribution: Conceptualization (equal) Formal analysis (equal) Investigation (equal) Supervision (supporting) Visualization (lead) Writing - original draft (equal) Contribution: Conceptualization (lead) Formal analysis (equal) Funding acquisition (lead) Project administration (lead) Supervision (lead) Validation (equal) Writing - original draft (equal) Writing - review & editing (lead)

The precise synthesis of miktoarm star polymers (MSPs) remains one of the great challenges in synthetic chemistry due to the difficulty in locating appropriate structural templates and polymer grafting/growing strategies with high selectivity and efficiency. Herein, ≈2 nm metal-organic polyhedra (MOPs), constructed from the coordination of isophthalic acid (IPA) and Cu 2+ , are applied as templates for the precise synthesis of 24-arm MSPs for their unique logarithmic ligand-exchange dynamics. Six different polymers are prepared with IPA as an end group and they further coordinated with Cu 2+ to afford the corresponding 24-arm star homo-polymers. MSPs can be obtained by mixing targeted homo-arm star polymers in solutions upon thermal annealing. The compositions of MSPs can be facilely and precisely tuned by the recipe of the star polymer mixtures used. Interestingly, the obtained MSPs can be sorted into homo-arm star polymers through a typical solvent extraction procedure. The hybridization and sorting process can be reversibly conducted through the cycle of thermal annealing and solvent treatment. The complex coordination framework not only opens new avenues for the facile and precise synthesis of MSPs and MOPs with hybrid functionalities, but also provides the capability to design sustainable polymer systems.

关键词： Inorganic–Organic Hybrid Materials Metal–Organic Polyhedra Miktoarm Star Polymers Solution Dynamics Sustainable Polymers

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Ligand-Assisted Coupling Manipulation for Efficient and Stable FAPbI3Colloidal Quantum Dot Solar Cells

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Angewandte Chemie 2022年第5期135卷

作者： Xuliang Zhang Hehe Huang Lujie Jin Chao Wen Qian Zhao Chenyu Zhao Junjun Guo Chen Cheng Hongshuai Wang Prof. Liang Zhang Prof. Youyong Li Prof. Yin Maung Maung Prof. Jianyu Yuan Prof. Wanli Ma Institute of Functional Nano & Soft Materials (FUNSOM) Soochow University Suzhou Jiangsu 215123 P. R. China Jiangsu Key Laboratory of Advanced Negative Carbon Technologies Soochow University Suzhou 215123 Jiangsu P. R. China Contribution: Conceptualization (equal) Data curation (lead) Investigation (lead) Writing - original draft (lead) Contribution: Data curation (equal) Formal analysis (supporting) Investigation (equal) Methodology (supporting) Writing - original draft (supporting) Jiangsu Key Laboratory for Carbon-Based Functional Materials and Devices Soochow University 199 Ren-Ai Road Suzhou Industrial Park Suzhou Jiangsu 215123 P. R. China Contribution: Data curation (supporting) Formal analysis (supporting) Investigation (supporting) Methodology (supporting) Writing - review & editing (supporting) Contribution: Investigation (supporting) Methodology (supporting) Writing - original draft (supporting) School of Materials Science and Engineering Nankai University Tianjin 300350 P. R. China Contribution: Conceptualization (supporting) Supervision (supporting) Writing - review & editing (supporting) Contribution: Data curation (supporting) Investigation (supporting) Contribution: Formal analysis (supporting) Investigation (supporting) Contribution: Data curation (supporting) Contribution: Supervision (supporting) Contribution: Resources (supporting) Supervision (supporting) Department of Physics University of Yangon Pyay Road Yangon 11181 Myanmar Contribution: Funding acquisition (supporting) Resources (supporting) Writing - review & editing (supporting) Contribution: Conceptualization (equal) Formal analysis (equal) Funding acquisition (lead) Resources (supporting) Writing - original draft (supporting) Writing - review & editing (lead)

For emerging perovskite quantum dots (QDs), understanding the surface features and their impact on the materials and devices is becoming increasingly urgent. In this family, hybrid FAPbI 3 QDs (FA: formamidium) exhibit higher ambient stability, near-infrared absorption and sufficient carrier lifetime. However, hybrid QDs suffer from difficulty in modulating surface ligand, which is essential for constructing conductive QD arrays for photovoltaics. Herein, assisted by an ionic liquid formamidine thiocyanate, we report a facile surface reconfiguration methodology to modulate surface and manipulate electronic coupling of FAPbI 3 QDs, which is exploited to enhance charge transport for fabricating high-quality QD arrays and photovoltaic devices. Finally, a record-high efficiency approaching 15 % is achieved for FAPbI 3 QD solar cells, and they retain over 80 % of the initial efficiency after aging in ambient environment (20–30 % humidity, 25 °C) for over 600 h.

关键词： Electronic Coupling FAPbI3 Ligand Perovskite Quantum Dot Solar Cells

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Evolutionary Algorithm Directed Synthesis of Mixed Anion Compounds LaF2X (X=Br, I) and LaFI2

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Angewandte Chemie 2023年第30期135卷

作者： Dr. Daichi Kato Dr. Peng Song Dr. Hiroki Ubukata Haruki Taguro Dr. Cédric Tassel Dr. Kohei Miyazaki Prof. Takeshi Abe Dr. Kousuke Nakano Prof. Kenta Hongo Prof. Ryo Maezono Prof. Hiroshi Kageyama Department of Energy and Hydrocarbon Chemistry Graduate School of Engineering Kyoto University Nishikyo-ku Kyoto 615-8510 Japan PRESTO Japan Science and Technology Agency (JST) Kawaguchi Saitama 332-0012 Japan Contribution: Data curation (lead) Formal analysis (lead) Funding acquisition (lead) Investigation (lead) Methodology (lead) Project administration (lead) Resources (supporting) Supervision (lead) Validation (equal) Visualization (equal) Writing - original draft (lead) Writing - review & editing (lead) School of Information Science JAIST Asahidai 1-1 Nomi Ishikawa 923-1292 Japan Contribution: Data curation (supporting) Formal analysis (supporting) Funding acquisition (supporting) Methodology (supporting) Software (supporting) Validation (supporting) Writing - original draft (supporting) Contribution: Formal analysis (supporting) Writing - original draft (supporting) Contribution: Data curation (supporting) Contribution: Data curation (supporting) Formal analysis (supporting) Writing - original draft (supporting) Contribution: Funding acquisition (supporting) Resources (supporting) Writing - original draft (supporting) Center for Basic Research on Materials (CBRM) National Institute for Materials Science (NIMS) 1-2-1 Sengen Tsukuba Ibaraki 305-0047 Japan Contribution: Writing - original draft (supporting) Research Center for Advanced Computing Infrastructure JAIST Asahidai 1-1 Nomi Ishikawa 923-1292 Japan Contribution: Conceptualization (lead) Funding acquisition (lead) Project administration (lead) Resources (lead) Supervision (lead) Validation (lead) Writing - original draft (supporting)

Mixed-anion compounds have attracted growing attentions, but their synthesis is challenging, making a rational search desirable. Here, we explored LaF 3 -LaX 3 (X=Cl, Br, I) system using ab initio structure searches based on evolutionary algorithms, and predicted LaF 2 X and LaFX 2 (X=Br, I), which are respectively isostructural with LaHBr 2 and YH 2 I, consisting of layered La-F blocks with single and double ordered honeycomb lattices, separated by van der Waals gaps. We successfully synthesized these compounds: LaF 2 Br and LaFI 2 crystallize in the predicted structure, while LaF 2 I is similar to the predicted one but with different layer stacking. LaF 2 I exhibits fluoride ion conductivity comparable to that of non-doped LaF 3 , and has the potential to show better ionic conductivity upon appropriate doping, given the theoretically lower diffusion energy barrier and the presence of soft iodine anions. This study shows the structure prediction using evolutionary algorithms will accelerate the discovery of mixed-anion compounds in future, in particular those with an ordered anion arrangement.

关键词： Evolutionary Algorithm Fluoride Ion Conductor Mixed Anion

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NaCdSb: An Orthorhombic Zintl Phase with Exceptional Intrinsic Thermoelectric Performance

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Angewandte Chemie 2022年第3期135卷

作者： Kai Guo Yuting Zhang Song Yuan Qinghang Tang Chen Lin Pengfei Luo Jiong Yang Shusheng Pan Li-Dong Zhao Guofeng Cheng Jiye Zhang Jun Luo School of Physics and Materials Science Guangzhou University Guangzhou 510006 China Research Center for Advanced Information Materials (CAIM) Huangpu Research & Graduate School of Guangzhou University Sino-Singapore Guangzhou Knowledge City Huangpu District Guangzhou 510555 China Contribution: Conceptualization (lead) Formal analysis (equal) Writing - original draft (lead) School of Materials Science and Engineering Shanghai University 99 Shangda Road Shanghai 200444 China Contribution: Data curation (equal) Investigation (equal) Validation (lead) Contribution: Data curation (lead) Formal analysis (equal) Materials Genome Institute Shanghai University 99 Shangda Road Shanghai 200444 China Key Laboratory of Artificial Micro- and Nano-Structures of Ministry of Education and School of Physics and Technology Wuhan University Wuhan 430072 China Contribution: Investigation (equal) Contribution: Investigation (equal) Methodology (supporting) Contribution: Investigation (equal) Writing - review & editing (supporting) School of Materials Science and Engineering Beihang University Beijing 100191 China Contribution: Methodology (equal) Writing - review & editing (equal) Analysis & Testing Center for Inorganic Materials Shanghai Institute of Ceramics Chinese Academy of Sciences Shanghai 200050 China Contribution: Formal analysis (equal) Investigation (supporting) Contribution: Data curation (equal) Writing - review & editing (supporting) Contribution: Supervision (lead) Writing - review & editing (equal)

Many Zintl phases are promising thermoelectric materials owning to their features like narrow band gaps, multiband behaviors, ideal charge transport tunnels, and loosely bound cations. Herein we show a new Zintl phase NaCdSb with exceptional intrinsic thermoelectric performance. Pristine NaCdSb exhibits semiconductor behaviors with an experimental hole concentration of 2.9×10 18 cm −3 and a calculated band gap of 0.5 eV. As the temperature increases, the hole concentration rises gradually and approaches its optimal one, leading to a high power factor of 11.56 μW cm −1 K −2 at 673 K. The ultralow thermal conductivity is derived from the small phonon group velocity and short phonon lifetime, ascribed to the structural anharmonicity of Cd−Sb bonds. As a consequence, a maximum zT of 1.3 at 673 K has been achieved without any doping optimization or structural modification, demonstrating that NaCdSb is a remarkable thermoelectric compound with great potential for performance improvement.

关键词： Electron-Crystal NaCdSb Phonon-Glass Thermoelectric Properties Zintl Phase

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Asymmetrically Substituted 10H,10′H-9,9′-Spirobi[acridine] Derivatives as Hole-Transporting Materials for Perovskite Solar Cells

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Angewandte Chemie 2022年第48期134卷

作者： Jianxing Xia Yi Zhang Marco Cavazzini Simonetta Orlandi Bin Ding Hiroyuki Kanda Nadja Klipfel Xiao-Xin Gao Qurat Ul Ain Vygintas Jankauskas Kasparas Rakstys Ruiyuan Hu Zeliang Qiu Abdullah M. Asiri Hobeom Kim Paul J. Dyson Gianluca Pozzi Mohammad Khaja Nazeeruddin Institute of Chemical Sciences and Engineering École Polytechnique Federale de Lausanne (EPFL) Lausanne 1015 Switzerland Contribution: Investigation (lead) Writing - original draft (lead) Contribution: Investigation (equal) Methodology (equal) CNR Institute of Chemical Sciences and Technologies “Giulio Natta” (CNR SCITEC) UOS Golgi via Golgi 19 20133 Milan Italy Contribution: Conceptualization (lead) Data curation (equal) Writing - review & editing (equal) Contribution: Conceptualization (equal) Data curation (equal) 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: Methodology (equal) Validation (equal) Contribution: Data curation (equal) Formal analysis (supporting) Institute of Chemical Physics Vilnius University Sauletekio al. 3 Vilnius 10257 Lithuania Department of Organic Chemistry Kaunas University of Technology Radvilenu pl. 19 Kaunas 50254 Lithuania New Energy Technology Engineering Laboratory of Jiangsu Province School of Science Nanjing University of Posts and Telecommunications (NJUPT) Nanjing 210023 China College of Materials and Chemistry and Chemical Engineering Chengdu University of Technology Chengdu Sichuan 610059 China Contribution: Formal analysis (equal) Writing - review & editing (equal) Center of Excellence for Advanced Materials Research (CEAMR) King Abdulaziz University P.O. Box 80203 21589 Jeddah Saudi Arabia Present address: School of Materials Science and Engineering Gwangju Institute of Science and Technology (GIST) Gwangju 61005 Republic of Korea Contribution: Conceptualization (equal) Writing - review & editing (equal) Contribution: Conceptualization (lead) Writing - review & editing (equal) Department of Materials Science and Engineering City University of Hong Kong Kowloon Hong Kong

Hole-transporting materials (HTMs) based on the 10 H , 10′ H -9,9′-spirobi [acridine] core ( BSA50 and BSA51 ) were synthesized, and their electronic properties were explored. Experimental and theoretical studies show that the presence of rigid 3,6-dimethoxy-9H-carbazole moieties in BSA 50 brings about improved hole mobility and higher work function compared to bis(4-methoxyphenyl)amine units in BSA51 , which increase interfacial hole transportation from perovskite to HTM. As a result, perovskite solar cells (PSCs) based on BSA50 boost power conversion efficiency (PCE) to 22.65 %, and a PSC module using BSA50 HTM exhibits a PCE of 21.35 % (6.5×7 cm) with a V oc of 8.761 V and FF of 79.1 %. The unencapsulated PSCs exhibit superior stability to devices employing spiro-OMeTAD, retaining nearly 90 % of their initial efficiency after 1000 h operation output. This work demonstrates the high potential of molecularly engineered spirobi[acridine] derivatives as HTMs as replacements for spiro-OMeTAD.

关键词： 3,6-Dimethoxy-9H-Carbazole Acridine Bis(4-Methoxyphenyl)Amine Acridine Hole Transporting Materials Perovskite Solar Cells Perovskite Solar Modules

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Correlation between Electrolyte Chemistry and Solid Electrolyte Interphase for Reversible Ca Metal Anodes

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Angewandte Chemie 2022年第50期134卷

作者： Dr. Zhen Hou Rui Zhou Yunduo Yao Zhiwen Min Dr. Ziheng Lu Prof. Ye Zhu Prof. Jean-Marie Tarascon Prof. Biao Zhang Department of Applied Physics & Research Institute for Smart Energy The Hong Kong Polytechnic University Hung Hom Hong Kong China Contribution: Conceptualization (equal) Data curation (lead) Formal analysis (lead) Investigation (lead) Methodology (equal) Validation (equal) Visualization (equal) Writing - original draft (lead) Writing - review & editing (equal) Contribution: Investigation (supporting) Shenzhen Institutes of Advanced Technology Chinese Academy of Sciences Shenzhen 518055 China Contribution: Software (supporting) Microsoft Research AI4Science Beijing 100080 China Contribution: Software (lead) Writing - review & editing (supporting) Chimie du Solide-Energie UMR 8260 Collège de France Paris France Contribution: Writing - review & editing (equal) Contribution: Conceptualization (equal) Funding acquisition (lead) Methodology (equal) Project administration (lead) Resources (lead) Supervision (lead) Validation (equal) Writing - review & editing (equal)

The development of rechargeable Ca metal batteries (RCMBs) is hindered by the Ca 2+ passivating solid electrolyte interphases (SEIs). The cation solvation structure dictated by electrolyte chemistry plays a critical role in the SEIs properties. While a relatively weak cation-solvent binding is preferred in Li metal anodes to promote anion-derived SEIs, we demonstrate an enhanced Ca deposition/stripping reversibility under a strong cation-solvent interaction, which is materialized in strongly-solvating solvent and highly-dissociated salt combinations. Such electrolyte formulations benefit the formation of solvent-occupied solvation structure and minimize the anion reduction, resulting in organic-rich/CaF 2 -poor SEIs for reversible Ca metal anodes. Furthermore, RCMBs paired with an organic cathode using the optimized electrolytes are demonstrated as a proof-of-concept. Our work reveals the paradigm shift in SEIs design for Ca metal anodes, opening up new opportunities for emerging RCMBs.

关键词： Ca Deposition/Stripping Electrolyte Formulation Solid Electrolyte Interphase Solvation Structure

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Metal Organic Framework Cubosomes

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Angewandte Chemie 2023年第11期135卷

作者： Chen Li Yi Pan Tianyu Xiao Luoxing Xiang Dr. Qian Li Dr. Feng Tian Prof. Ian Manners Prof. Yiyong Mai School of Chemistry and Chemical Engineering Frontiers Science Center for Transformative Molecules Shanghai Key Laboratory of Electrical Insulation and Thermal Ageing Shanghai Jiao Tong University 800 Dongchuan Road Shanghai 200240 China Department of Chemistry Centre for Advanced Materials and Related Technology (CAMTEC) University of Victoria 3800 Finnerty Road Victoria BC V8P 5C2 Canada Contribution: Data curation (lead) Formal analysis (lead) Investigation (lead) Writing - original draft (lead) Writing - review & editing (lead) Contribution: Data curation (equal) Formal analysis (equal) Investigation (equal) Writing - original draft (equal) Writing - review & editing (equal) Contribution: Data curation (supporting) Investigation (supporting) Writing - original draft (supporting) Contribution: Data curation (supporting) Formal analysis (supporting) Investigation (supporting) Contribution: Data curation (supporting) Formal analysis (supporting) Shanghai Synchrotron Radiation Facility Zhangjiang Lab Shanghai Advanced Research Institute Chinese Academy of Sciences 239 Zhangheng Road Shanghai 201204 China Contribution: Data curation (supporting) Formal analysis (supporting) Writing - original draft (supporting) Contribution: Conceptualization (supporting) Funding acquisition (supporting) Project administration (equal) Supervision (equal) Writing - original draft (supporting) Writing - review & editing (supporting) Contribution: Conceptualization (lead) Data curation (supporting) Formal analysis (lead) Funding acquisition (lead) Investigation (supporting) Methodology (lead) Project administration (lead) Supervision (lead) Writing - original draft (lead) Writing - review & editing (lead)

We demonstrate a general strategy for the synthesis of ordered bicontinuous-structured metal organic frameworks (MOFs) by using polymer cubosomes (PCs) with a double primitive structure ( Im m symmetry) as the template. The filling of MOF precursors in the open channel of PCs, followed by their coordination and removal of the template, generates MOF cubosomes with a single primitive topology ( Pm m ) and average mesopore diameters of 60–65 nm. Mechanism study reveals that the formation of ZIF-8 cubosomes undergoes a new MOF growth process, which involves the formation of individual MOF seeds in the template, their growth and eventual fusion into the cubosomes. Their growth kinetics follows the Avrami equation with an Avrami exponent of n =3 and a growth rate of k =1.33×10 −4 , indicating their fast 3D heterogeneous growth mode. Serving as a bioreactor, the ZIF-8 cubosomes show high loading of trypsin enzyme, leading to a high catalytic activity in the proteolysis of bovine serum albumin.

关键词： Bicontinuous Structure Block Copolymer Cubosome Metal Organic Framework Proteolysis

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Wide-Bandgap Perovskite Solar Cell Using a Fluoride-Assisted Surface Gradient Passivation Strategy

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Angewandte Chemie 2023年第11期135卷

作者： Nan Yan Yan Gao Junjie Yang Zhimin Fang Jiangshan Feng Prof. Xiaojun Wu Prof. Tao Chen Prof. Shengzhong (Frank) 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 School of Materials Science and Engineering Shaanxi Normal University Xi'an 710119 China Contribution: Data curation (lead) Formal analysis (lead) Investigation (lead) Methodology (lead) Writing - original draft (lead) Writing - review & editing (lead) Hefei National Laboratory for Physical Sciences at Microscale Department of Materials Science and Engineering University of Science and Technology of China Hefei 230026 China Contribution: Software (lead) Contribution: Methodology (equal) Validation (supporting) Contribution: Formal analysis (equal) Funding acquisition (lead) Investigation (equal) Writing - original draft (equal) Writing - review & editing (equal) Contribution: Funding acquisition (supporting) Investigation (supporting) Writing - original draft (equal) Writing - review & editing (equal) Dalian National Laboratory for Clean Energy iChEM Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian 116023 China Contribution: Formal analysis (supporting) Funding acquisition (lead) Investigation (equal) Project administration (lead) Resources (lead) Supervision (lead) Writing - original draft (supporting) Writing - review & editing (supporting)

Wide-band gap (1.68 eV) perovskite solar cells (PSCs) are important components of perovskite/Si tandem devices. However, the efficiency of wide band gap PSCs has been limited by their huge open-circuit voltage ( V oc ) deficit due to non-radiative recombination. Deep-level acceptor defects are identified as the major killers of V oc , and they can be effectively improved by passivation with ammonium salts. Theoretical calculation predicts that increasing the distance between F and −NH 3 + of fluorinated ammonium can dramatically enhance the electropositivity of −NH 3 + terminals, thus providing strong adsorption onto the negatively charged I A and I Pb anti-site defects. Characterizations further confirm that surface gradient passivation employing p -FPEAI demonstrates the most efficient passivation effect. Consequently, a record-efficiency of 21.63 % with the smallest V oc deficit of 441 mV is achieved for 1.68 eV-band gap inverted PSCs. Additionally, a flexible PSC and 1 cm 2 opaque device also deliver the highest PCEs of 21.02 % and 19.31 %, respectively.

关键词： Defects Fluoride Open-Circuit Voltage Deficit Perovskite Wide Band Gap

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