检索结果-内蒙古大学图书馆

engineering residues on C interface to improve thermostability of nitrilase for biosynthesis of Pregabalin precursor

引用

AIChE Journal 2023年第11期69卷

作者： Xia-Feng Lu Xiao-Ling Tang Chen-Hui Xu Hong-Juan Diao Zhe-Ming Wu Ren-Chao Zheng Yu-Guo Zheng Key Laboratory of Bioorganic Synthesis of Zhejiang Province College of Biotechnology and Bioengineering Zhejiang University of Technology Hangzhou People's Republic of China Engineering Research Center of Bioconversion and Biopurification of Ministry of Education Zhejiang University of Technology Hangzhou People's Republic of China Contribution: Investigation (lead) Methodology (supporting) Writing - original draft (lead) Contribution: Formal analysis (supporting) Investigation (supporting) Writing - original draft (supporting) Contribution: Data curation (supporting) Formal analysis (supporting) Contribution: Formal analysis (lead) Contribution: Data curation (supporting) Contribution: Conceptualization (lead) Funding acquisition (lead) Project administration (lead) Supervision (lead) Contribution: Project administration (supporting) Supervision (supporting)

Nitrilase-mediated bioprocesses exhibited great potential in the production of value-added carboxylic acids. However, poor thermostability of nitrilases usually restricts their industrial applications. Herein, the thermostability of nitrilase Ba NIT M0 was significantly improved by engineering the amino acid residues on the intersection of two dimers (C interface). Except for simultaneous enhancement of enantioselectivity and activity, the best variant V82L/M127I/L159M/F166Q/C237S/Q260H ( Ba NIT M4 ) showed a 10.8-fold increase in half-life at 30°C compared with Ba NIT M0 . Structural analysis demonstrated that additional hydrogen bonds were formed between the residues on the C interface, which strengthened the interactions of two symmetrical regions and spirals. Subsequently, the engineered nitrilase was immobilized onto epoxy resins LXTE-603 and the immobilized nitrilase exhibited excellent stability over 12 repeated cycles, which indicated a great industrial potential for biosynthesis of Pregabalin precursor.

关键词： C interface immobilized nitrilase Pregabalin precursor protein engineering thermostability

来源：评论

学校读者我要写书评

暂无评论

Favoring CO Intermediate Stabilization and Protonation by Crown Ether for CO2Electromethanation in Acidic Media

引用

Angewandte Chemie 2023年第50期135卷

作者： Keqiang Xu Jinhan Li Fangming Liu Xijie Chen Tete Zhao Fangyi Cheng Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education) Engineering Research Center on High-Efficiency Energy Storage (Ministry of Education) Renewable Energy Conversion and Storage Center College of Chemistry Nankai University Tianjin 300071 China Contribution: Data curation (lead) Formal analysis (lead) Investigation (lead) Methodology (lead) Visualization (lead) Writing - original draft (equal) Contribution: Data curation (supporting) Formal analysis (equal) Investigation (supporting) Methodology (equal) Software (equal) Validation (equal) Frontiers Science Center for New Organic Matter Nankai University Tianjin 300071 China Contribution: Formal analysis (equal) Funding acquisition (supporting) Methodology (equal) Project administration (lead) Validation (supporting) Writing - review & editing (lead) Contribution: Data curation (supporting) Formal analysis (supporting) Investigation (supporting) Methodology (supporting) Validation (supporting) Contribution: Data curation (supporting) Formal analysis (supporting) Investigation (supporting) Visualization (supporting) Haihe Laboratory of Sustainable Chemical Transformations Tianjin 300192 China Contribution: Conceptualization (lead) Formal analysis (equal) Methodology (equal) Resources (lead) Supervision (lead) Writing - review & editing (equal)

The large-scale deployment of CO 2 electroreduction is hampered by deficient carbon utilization in neutral and alkaline electrolytes due to CO 2 loss into (bi)carbonates. Switching to acidic media mitigates carbonation, but suffers from low product selectivity because of hydrogen evolution. Here we report a crown ether decoration strategy on a Cu catalyst to enhance carbon utilization and selectivity of CO 2 methanation under acidic conditions. Macrocyclic 18-Crown-6 is found to enrich potassium cations near the Cu electrode surface, simultaneously enhancing the interfacial electric field to stabilize the *CO intermediate and accelerate water dissociation to boost *CO protonation. Remarkably, the mixture of 18-Crown-6 and Cu nanoparticles affords a CH 4 Faradaic efficiency of 51.2 % and a single pass carbon efficiency of 43.0 % toward CO 2 electroreduction in electrolyte with pH=2. This study provides a facile strategy to promote CH 4 selectivity and carbon utilization by modifying Cu catalysts with supramolecules.

关键词： CO2 Electroreduction Copper Catalyst Crown Ether Methanation Protonation

来源：评论

学校读者我要写书评

暂无评论

Cooperative Catalysis of Polysulfides in Lithium-Sulfur Batteries through Adsorption Competition by Tuning Cationic Geometric Configuration of Dual-active Sites in Spinel Oxides

引用

Angewandte Chemie 2022年第8期135卷

作者： Dr. Hongtai Li Pei Shi Lei Wang Tianran Yan Tong Guo Xiao Xia Prof. Chi Chen Prof. Jing Mao Prof. Dan Sun Prof. Liang Zhang Institute of Functional Nano & Soft Materials (FUNSOM) Soochow University Suzhou 215123 China Contribution: Conceptualization (lead) Formal analysis (lead) Writing - original draft (lead) CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Key Laboratory of Nanomaterials Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou 350002 China Xiamen Institute of Rare Earth Materials Haixi Institute Chinese Academy of Sciences Xiamen 361021 China Contribution: Data curation (lead) Investigation (equal) Contribution: Investigation (equal) Validation (equal) Contribution: Investigation (equal) Key Laboratory for Soft Chemistry and Functional Materials of Ministry of Education Nanjing University of Science and Technology Nanjing 210094 China Contribution: Data curation (equal) Investigation (equal) School of Materials Science and Engineering Zhengzhou University Zhengzhou 450001 China Contribution: Investigation (equal) Supervision (equal) Jiangsu Key Laboratory of Advanced Negative Carbon Technologies Soochow University Suzhou 215123 China Contribution: Conceptualization (lead) Funding acquisition (lead) Supervision (lead) Writing - review & editing (lead)

来源：评论

学校读者我要写书评

暂无评论

Solid–Liquid Interfacial Coordination Chemistry Enables High-Capacity Ammonium Storage in Amorphous Manganese Phosphate

引用

Angewandte Chemie 2022年第37期134卷

作者： Duo Yang Prof. Yu Song Ming-Yue Zhang Zengming Qin Jie Liu Prof. Xiao-Xia Liu Department of Chemistry Northeastern University 3-11 Wenhua Road Heping district Shenyang 110819 China School of Resources and Civil Engineering Northeastern University 3-11 Wenhua Road Heping district Shenyang 110819 China National-local Joint Engineering Research Center of High-efficient Exploitation Technology for Refractory Iron Ore Resources Shenyang 110819 Liaoning China National Frontiers Science Center for Industrial Intelligence and Systems Optimization Northeastern University 3-11 Wenhua Road Heping district Shenyang 110819 China Key Laboratory of Data Analytics and Optimization for Smart Industry Northeastern University) Ministry of Education China 3-11 Wenhua Road Heping district Shenyang 110819 China

Ammonium (NH 4 + ) ion as charge carrier is attracting attention in aqueous batteries. Yet, most NH 4 + host materials are still limited by the relatively low capacities. Here, we fabricated a manganese phosphate (MP-20) for NH 4 + ion storage. MP-20 displays a high capacity of 299.6 mAh g −1 at 1 A g −1 in ammonium acetate (NH 4 Ac) electrolyte, outperforming other reported NH 4 + host materials. Spectroscopy studies suggest a new NH 4 + /H + co-insertion mechanism. We surprisingly discover that the NH 4 Ac electrolyte plays an important role in improving the charge storage capability of the materials. Experimental and computational results indicate acetate ions can form coordination bonds with the Mn atoms, tailoring the electronic structure of the Mn atoms and the surrounding O atoms, and therefore facilitating the NH 4 + storage process. Our findings provide a new NH 4 + host material and propose the important role of the electrolyte-electrode coordination effect in aqueous ammonium batteries.

关键词： Aqueous Ammonium-Ion Batteries Charge Storage Mechanism Coordination Electrochemical Deposition Manganese Phosphate

来源：评论

学校读者我要写书评

暂无评论

Distinguishing Protein Chemical Topologies Using Supercharging Ion Mobility Spectrometry-Mass Spectrometry

引用

Angewandte Chemie 2023年第51期135卷

作者： Jiyeon Lee Dahye Im Yajie Liu Jing Fang Xibao Tian Minsu Kim Prof. Wen-Bin Zhang Prof. Jongcheol Seo Department of Chemistry Pohang University of Science and Technology (POSTECH) 77 Cheongam-ro Nam-gu Pohang 37673 Gyeonsangbuk-do (Republic of Korea Contribution: Data curation (lead) Formal analysis (equal) Visualization (lead) Writing - original draft (lead) Writing - review & editing (supporting) Contribution: Data curation (supporting) Formal analysis (equal) Visualization (supporting) Writing - original draft (supporting) Writing - review & editing (supporting) Beijing National Laboratory for Molecular Sciences Key Laboratory of Polymer Chemistry & Physics of Ministry of Education Center for Soft Matter Science and Engineering College of Chemistry and Molecular Engineering Peking University Beijing 100871 P. R. China Contribution: Resources (equal) Contribution: Data curation (supporting) Validation (supporting) Contribution: Conceptualization (equal) Funding acquisition (equal) Investigation (equal) Project administration (supporting) Writing - review & editing (equal) Contribution: Conceptualization (equal) Funding acquisition (equal) Investigation (lead) Project administration (lead) Validation (lead) Writing - review & editing (lead)

A technique combining ion mobility spectrometry-mass spectrometry (IMS-MS) and supercharging electrospray ionization (ESI) has been demonstrated to differentiate protein chemical topology effectively. Incorporating as many charges as possible into proteins via supercharging ESI allows the protein chains to be largely unfolded and stretched, revealing their hidden chemical topology. Different chemical topologies result in differing geometrical sizes of the unfolded proteins due to constraints in torsional rotations in cyclic domains. By introducing new topological indices, such as the chain-length-normalized collision cross-section (CCS) and the maximum charge state ( z M ) in the extensively unfolded state, we were able to successfully differentiate various protein chemical topologies, including linear chains, ring-containing topologies (lasso, tadpole, multicyclics, etc.), and mechanically interlocked rings, like catenanes.

关键词： Mass Spectrometry Protein engineering Proteins

来源：评论

学校读者我要写书评

暂无评论

Managing Multiple Halide-Related Defects for Efficient and Stable Inorganic Perovskite Solar Cells

引用

Angewandte Chemie 2023年第30期135卷

作者： Zhiteng Wang Prof. Qingwen Tian Hao Zhang Prof. Huidong Xie Yachao Du Lei Liu Xiaolong Feng Adel Najar Xiaodong Ren 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 P. R. China Contribution: Conceptualization (lead) Data curation (lead) Formal analysis (lead) Investigation (lead) Contribution: Conceptualization (lead) Funding acquisition (lead) Project administration (lead) Supervision (lead) Validation (lead) Writing - original draft (lead) Writing - review & editing (lead) Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of Sciences Beijing 100049 P. R. China Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian 116023 P. R. China Contribution: Data curation (supporting) Formal analysis (supporting) Investigation (supporting) School of Chemistry and Chemical Engineering Xi'an University of Architecture and Technology Xi'an 710055 P. R. China Contribution: Formal analysis (supporting) Validation (supporting) Contribution: Data curation (supporting) Formal analysis (supporting) Contribution: Data curation (supporting) Formal analysis (supporting) Methodology (supporting) Resources (supporting) Department of Physics College of Science United Arab Emirates University Al Ain 15551 United Arab Emirates Contribution: Supervision (supporting) Validation (supporting) Writing - review & editing (supporting) Contribution: Data curation (supporting) Formal analysis (supporting) Methodology (supporting) Contribution: Funding acquisition (lead) Project administration (lead) Validation (lead) Writing - review & editing (lead)

Halide-related surface defects on inorganic halide perovskite not only induce charge recombination but also severely limit the long-term stability of perovskite solar cells. Herein, adopting density functional theory calculation, we verify that iodine interstitials (I i ) has a low formation energy similar to that of the iodine vacancy (V I ) and is also readily formed on the surface of all-inorganic perovskite, and it is regarded to function as an electron trap. We screen a specific 2,6-diaminopyridine (2,6-DAPy) passivator, which, with the aid of the combined effects from halogen-N pyridine and coordination bonds, not only successfully eliminates the I i and dissociative I 2 but also passivates the abundant V I . Furthermore, the two symmetric neighboring -NH 2 groups interact with adjacent halides of the octahedral cluster by forming hydrogen bonds, which further promotes the adsorption of 2,6-DAPy molecules onto the perovskite surface. Such synergetic effects can significantly passivate harmful iodine-related defects and undercoordinated Pb 2+ , prolong carrier lifetimes and facilitate the interfacial hole transfer. Consequently, these merits enhance the power-conversion efficiency (PCE) from 19.6 % to 21.8 %, the highest value for this type of solar cells, just as importantly, the 2,6-DAPy-treated CsPbI 3− x Br x films show better environmental stability.

关键词： All-Inorganic Perovskite CsPbI3−xBrx Defect Passivation Iodine-Related Defects Solar Cells

来源：评论

学校读者我要写书评

暂无评论

Dual-Network Structured Hydrogel Electrolytes Engaged Solid-State Rechargeable Zn-Air/Iodide Hybrid Batteries

引用

Angewandte Chemie 2022年第44期134卷

作者： Qingqing Liu Chenfeng Xia Chaohui He Wei Guo Zi Ping Wu Zhen Li Qiang Zhao Bao Yu Xia Key Laboratory of Material Chemistry for Energy Conversion and Storage (Ministry of Education) Hubei Key Laboratory of Material Chemistry and Service Failure School of Chemistry and Chemical Engineering Huazhong University of Science and Technology (HUST) 1037 Luoyu Rd Wuhan 430074 PR China Contribution: Conceptualization (lead) Data curation (lead) Investigation (lead) Validation (lead) Visualization (lead) Writing - original draft (lead) Writing - review & editing (equal) Contribution: Investigation (equal) Methodology (supporting) Validation (equal) Writing - original draft (equal) Contribution: Methodology (equal) Validation (equal) Contribution: Project administration (equal) Supervision (equal) Visualization (equal) School of Materials Science and Engineering Jiangxi University of Science and Technology (JXUST) Ganzhou 341000 PR China Contribution: Funding acquisition (equal) Project administration (equal) Resources (supporting) State Key Laboratory of Material Processing and Die & Mold Technology School of Materials Science and Engineering Huazhong University of Science and Technology 1037 Luoyu Rd Wuhan 430074 PR China Contribution: Resources (supporting) Validation (supporting) Writing - review & editing (supporting) Contribution: Data curation (supporting) Resources (supporting) Validation (supporting) Contribution: Conceptualization (lead) Project administration (lead) Supervision (lead) Writing - original draft (equal) Writing - review & editing (equal)

As a key component of batteries, the electrolyte determines the ion transport and interface chemistry of the cathode and anode. In this work, we develop a dual-network structured hydrogel electrolyte composed of polyacrylamide (PAM), sodium alginate (SA) and potassium iodide (KI) for solid-state zinc-air/iodide hybrid batteries. The assembled hybrid battery shows excellent renewability and a long cycling life of 110 h with a high energy efficiency of 80 %. The ion-crosslinked dual-network structure endows the material with improved mechanical strength and increased ionic conductivity. More importantly, the introduction of iodine species not only offers more favorable cathodic kinetics of iodide/iodate redox than oxygen electrocatalysis but also regulates the solvation structure of zinc ions to ensure better interface stability. This work provides significant concepts for developing novel solid-state electrolytes to realize high-performance energy devices and technologies.

关键词： Hydrogel Electrolyte Iodide/Iodate Redox Oxygen Electrocatalysis Solid-State Battery Solvation Effect

来源：评论

学校读者我要写书评

暂无评论

Electron Acceptor Molecule Doping Induced π–π Interaction to Promote Charge Transport Kinetics for Efficient and Stable 2D/3D Perovskite Solar Cells

引用

Angewandte Chemie 2023年第26期135卷

作者： Lian Wang Bohong Chang Hui Li Yutong Wu Luyuan Zhang Longwei Yin Key Laboratory for Liquid-Solid Structural Evolution and Processing of Materials Ministry of Education School of Materials Science and Engineering Shandong University 250061 Jinan P. R.China Contribution: Conceptualization (lead) Data curation (lead) Formal analysis (lead) Investigation (lead) Methodology (lead) Writing - original draft (lead) Contribution: Data curation (supporting) Investigation (supporting) Methodology (supporting) Writing - original draft (supporting) Contribution: Formal analysis (supporting) Investigation (supporting) Methodology (supporting) Writing - original draft (supporting) Contribution: Conceptualization (supporting) Methodology (supporting) Writing - original draft (supporting) Contribution: Formal analysis (supporting) Investigation (supporting) Writing - original draft (supporting) Contribution: Conceptualization (lead) Data curation (lead) Funding acquisition (lead) Investigation (lead) Methodology (lead) Writing - original draft (lead)

Although the incorporation of 2D perovskite into 3D perovskite can greatly enhance intrinsic stability, power conversion efficiency (PCE) of 2D/3D perovskite is still inferior to its 3D counterpart due to poor carrier transport kinetics resulted from the quantum and dielectric confinement of 2D component. To overcome this issue, the electron acceptor molecule 1,2,4,5-tetracyanobenzene (TCNB) was introduced to trigger intermolecular π–π interaction in 2D perovskite along with the electronic doping of 2D/3D perovskite to improve charge transfer efficiency. By virtue of high electron affinity, TCNB can undergo electron transfer reaction and subsequently establish π–π interaction with 1-naphthalenemethylammonium (NMA) cations, greatly strengthening lattice rigidity and reducing exciton binding energy. Transmission electron microscopy results demonstrate that 2D phases are mainly distributed at grain boundaries, reducing defect density and weakening nonradiative recombination. Meanwhile, the p-type doping of perovskite by TCNB optimizes energy level alignment at perovskite/hole transport layer interface. Consequently, PCE of champion device is significantly boosted to 24.01 %. The unencapsulated device retains an initial efficiency close to 94 % after exposure to ambient environment for over 1000 h. This work paves a novel path for designing new mixed-dimensional perovskite solar cells with high PCE and superior stability.

关键词： 2D/3D Perovskite Charge Transport Electron Acceptor Molecule Solar Cells π–π Interaction

来源：评论

学校读者我要写书评

暂无评论

Virus Detection: Nanopore Targeted Sequencing for the Accurate and Comprehensive Detection of SARS-CoV-2 and Other Respiratory Viruses (Small 32/2020)

引用

Small 2020年第32期16卷

作者： Ming Wang Aisi Fu Ben Hu Yongqing Tong Ran Liu Zhen Liu Jiashuang Gu Bin Xiang Jianghao Liu Wen Jiang Gaigai Shen Wanxu Zhao Dong Men Zixin Deng Lilei Yu Wu Wei Yan Li Tiangang Liu Department of Clinical Laboratory Renmin Hospital of Wuhan University Wuhan 430060 China Key Laboratory of Combinatorial Biosynthesis and Drug Discovery Ministry of Education and Wuhan University School of Pharmaceutical Sciences Wuhan 430071 China CAS Key Laboratory of Computational Biology CAS-MPG Partner Institute for Computational Biology Shanghai Institute of Nutrition and Health University of Chinese Academy of Sciences Chinese Academy of Sciences Shanghai 200031 China Wuhan Dgensee Clinical Laboratory Co. Ltd. Wuhan 430075 China Wuhan Institute of Virology Chinese Academy of Sciences Wuhan 430071 China Department of Internal Medicine Renmin Hospital of Wuhan University Wuhan 430060 China Center for Biomedical Informatics Shanghai Engineering Research Center for Big Data in Pediatric Precision Medicine Shanghai Children's Hospital Shanghai Jiao Tong University Shanghai 200040 China

来源：评论

学校读者我要写书评

暂无评论

Bidirectional Tandem Electrocatalysis Manipulated Sulfur Speciation Pathway for High-Capacity and Stable Na-S Battery

引用

Angewandte Chemie 2022年第6期135卷

作者： Hong Zhang Bin Song Weiwei Zhang Bowen An Lin Fu Songtao Lu Yingwen Cheng Qianwang Chen Ke Lu Institutes of Physical Science and Information Technology School of Materials Science and Engineering Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of Education Anhui University Hefei Anhui 230601 China Hefei National Laboratory for Physical Sciences at the Microscale University of Science and Technology of China Hefei Anhui 230026 China Contribution: Conceptualization (equal) Writing - original draft (equal) Institute of Functional Nano & Soft Materials (FUNSOM) Soochow University Suzhou Jiangsu 215123 China Contribution: Data curation (supporting) Formal analysis (supporting) Writing - original draft (supporting) School of Chemistry and Chemical Engineering Qufu Normal University Qufu Shandong 273165 China School of Chemistry and Chemical Engineering Harbin Institute of Technology Harbin Heilongjiang 150001 China Contribution: Data curation (supporting) Investigation (supporting) Department of Chemistry and Biochemistry Northern Illinois University DeKalb IL 60115 USA Contribution: Formal analysis (supporting) School of Chemistry and Chemical Engineering Guizhou University Guiyang Guizhou 550025 China Contribution: Formal analysis (supporting) Writing - review & editing (supporting) Contribution: Data curation (supporting) Investigation (supporting) Writing - review & editing (supporting) Contribution: Writing - review & editing (equal) Contribution: Conceptualization (lead) Formal analysis (lead) Writing - original draft (lead) Writing - review & editing (lead)

The sluggish polysulfide redox kinetics and the uncontrollable sulfur speciation pathway, leading to serious shuttling effect and high activation barrier associated with sulfur cathode. We describe here the use of core–shell structured composite matrixes containing abundant catalytic sites for nearly fully reversible cycling of sulfur cathodes for Na-S batteries. The bidirectional tandem electrocatalysis provide successive reversible conversion of both long- and short-chain polysulfides, whereas Fe 2 O 3 accelerates Na 2 S 8 /Na 2 S 6 to Na 2 S 4 conversion and the redox-active Fe(CN) 6 4− -doped polypyrrole shell catalyzes Na 2 S 4 reduction to Na 2 S. The electrochemically reactive Na 2 S can be readily charged back to sulfur with minimal overpotential. Simultaneously, stable cycling of Na-S pouch cell with a high reversible capacity of 696 mAh g −1 is also demonstrated. The bidirectional confined tandem catalysis renders the manipulation of sulfur redox electrochemistry for practical Na-S cells.

关键词： Bidirectional Catalysts Confined Catalysis Na-S Battery Polysulfide Manipulation

来源：评论

学校读者我要写书评

暂无评论

建议与咨询留下您的常用邮箱和电话号码，以便我们向您反馈解决方案和替代方法

时间限定

文献类型

馆藏选择

核心期刊

语言

文献类型

帮助

文字说明：

检索规则说明：

检索范例：

分类表

所选分类

限定检索结果

文献类型

馆藏范围

日期分布

学科分类号

主题

机构

作者

语言

请选择保存的检索档案：

请选择收藏分类：

通借通还

建议与咨询 留下您的常用邮箱和电话号码，以便我们向您反馈解决方案和替代方法

时间限定

文献类型

馆藏选择

核心期刊

语言

文献类型

帮助

文字说明：

检索规则说明：

检索范例：

分类表

所选分类

限定检索结果

文献类型

馆藏范围

日期分布

学科分类号

主题

机构

作者

语言

请选择保存的检索档案： 新增检索档案 确定 取消

请选择收藏分类： 新增自定义分类 确定 取消

通借通还

建议与咨询留下您的常用邮箱和电话号码，以便我们向您反馈解决方案和替代方法

请选择保存的检索档案：

请选择收藏分类：