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IRC analysis of methanol carbonylation reaction catalyzed by rhodium complex

science china Chemistry 2004年第1期47卷 41-49页

作者： hao maorong, feng wenlin, jl yongqiang & lei mingfaculty of science, beijing university of chemical engineering, beijing 100029, china Faculty of chemical engineering, Ningxia university, Yinchuan 750021, china Faculty of science Beijing University of Chemical Engineering Beijing China Faculty of chemical engineering Ningxia University Yinchuan China

In the reaction cycle for methanol carbonylation catalyzed by Rh complex, the structure geometries of the reactant, intermediates, transition states and product of each elemental reaction have been studied by using the energy gradient method at HF/LANL2DZ level, and the changes of their potential profiles have also been calculated. Through IRC analyses of the transition states for each elemental reaction, it is confirmed that the various structure geometries obtained are stationary points on the cycle reaction pathway of methanol carbonylation catalyzed by Rh complex, and the changes are given in energies and structure geometries of the reactant molecules along the reaction pathway of lowest energy. It has been proposed that the geometrical conversions of intermediates play an important role during the cycle reaction. Through analyses of structure geometries, it has been suggested that, in addition to cis- and trans- structure exchange linkage of catalysis reactive species, the two pathways, cis- and trans-cata- lyzed cycle reactions, can also be linked through geometrical conversion of intermediates, of which the activation energy is 49.79 kJ/mol. Moreover, the reductive elimination elemental reaction may be neither cis-cycle nor trans- one, showing that the cycle reaction can be achieved through various pathways. However different the pathway, the oxidative addition elemental reaction of CH3I is the rate-controlling step.

关键词： rhodium complex catalyst, methanol carbonylation, ab initio method, homogeneous catalysis.

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Screened peptides from one-bead one-compound technique extend half-life of peptide drugs in circulation through binding to albumin

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Chinese chemical Letters 2024年第3期35卷 384-388页

作者： Yi-Jing Li Lingze Zhang Ming-hao Pang Pei-Pei Yang Lu-Ming Guo Kuo Zhang Da-Yong Hou lei Wang hao Wang Hui Cao State Key Laboratory for Advanced Metals and Materials School of Materials Science and EngineeringUniversity of Science and Technology BeijingBeijing 100083China CAS Center for Excellence in Nanoscience CAS Key Laboratory for Biomedical Effects of Nanomaterials NanosafetyNational Center for Nanoscience and Technology(NCNST)Beijing 100190China

Peptide drugs are known for their high biological ***,compared with small molecule drugs,peptide drugs are easily oxidized and hydrolyzed as well as short in ***,inspired by the long circulation of albumin in blood,we screened albumin binding peptides(ABPs)from a one-bead one-compound(OBOC)peptide library to increase the half-life of peptide *** displaying random peptides were screened using fluorescent labeled human serum *** beads with specific binding to albumin were isolated for *** selected ABPs can effectively bind to albumin,thus possessing the long circulation of *** dissociation constant(K_(D))of ABPs to albumin is up to 1×10^(-8)mol/*** one of ABPs(ABP2)was coupled to triptorelin,the circulation half-life of triptorelin in mice was significantly prolonged to 263.50 h much longer than that of triptorelin alone(179.07 h).In addition,the combination therapy using ABP-conjugated triptorelin and doxorubicin(DOX)can effectively inhibit the proliferation of tumor cells in *** OBOC screening strategy and resulting ABPs showed great potential for enhancing the delivery efficiency of peptide drugs.

关键词： One-bead one-compound Combinatorial library Albumin binding Drug delivery Triptorelin

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Selenopeptide nanomedicine ameliorates atherosclerosis by reducing monocyte adhesions and inflammations

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Nano Research 2024年第7期17卷 6332-6341页

作者： Zhen Luo Yuxing Jiang Zimo Liu Lamei Guo Li Zhang Hongtao Rong Zhongyu Duan Hongwen Liang Aili Zhang lei Wang Yu Yi hao Wang CAS Center for Excellence in Nanoscience CAS Key Laboratory for Biomedical Effects of Nanomaterials and NanosafetyNational Center for Nanoscience and Technology(NCNST)No.11 BeiyitiaoZhongguancunBeijing 100190China School of chemical engineering and Technology Hebei University of TechnologyTianjin 300130China Tianjin Medical university General Hospital Tianjin 300052China university of Chinese Academy of sciences Beijing 100049China School of Environmental science and Safety engineering Tianjin University of TechnologyTianjin 300384China College of Pharmacy Chongqing Medical UniversityChongqing 400016China School of Biomedical engineering Shanghai Jiao Tong UniversityShanghai 200240China

Atherosclerosis is an inflammatory disease that may cause severe heart disease and *** pharmacotherapy for atherosclerosis shows limited *** the progression of atherosclerosis,monocyte adhesions and inflammatory macrophages play vital ***,precise regulations of inflammatory immune microenvironments in pathological tissues remain ***,we report an atherosclerotic plaque-targeted selenopeptide nanomedicine for inhibiting atherosclerosis progression by reducing monocyte adhesions and inflammation of *** targeted nanomedicine has 2.2-fold enhancement in atherosclerotic lesion *** oxidation-responsibility of selenopeptide enables eliminations of reactive oxygen species and specific release of anti-inflammatory drugs,thereby reducing inflammation responses of ***,we find the oxidative metabolite of selenopeptide,octadecyl selenite,can bind to P-selectin in a high affinity with a dissociation constant of 1.5μ*** in situ generated active seleno-species further inhibit monocyte adhesions for anti-inflammation in *** local regulations of monocyte adhesions and inflammations,the selenopeptide nanomedicine achieves 2.6-fold improvement in atherosclerotic plaque inhibition compared with simvastatin in the atherosclerosis mouse ***,the selenopeptide nanomedicine also displays excellent biological safety in both mice and rhesus *** study provides a safe and effective platform for regulating inflammatory immune microenvironments for inflammatory diseases such as atherosclerosis.

关键词： selenopeptide self-assembly atherosclerosis monocyte adhesion anti-inflammation

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Radical innovation breakthroughs of biodegradation of plastics by insects:history,present and future perspectives

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Frontiers of Environmental science & engineering 2024年第6期18卷 127-165页

作者： Shan-Shan Yang Wei-Min Wu Federica Bertocchini Mark Eric Benbow Suja P.Devipriya Hyung Joon Cha Bo-Yu Peng Meng-Qi Ding lei He Mei-Xi Li Chen-hao Cui Shao-Nan Shi Han-Jun Sun Ji-Wei Pang Defu He Yalei Zhang Jun Yang Deyi Hou De-feng Xing Nan-Qi Ren Jie Ding Craig S.Criddle State Key Laboratory of Urban Water Resource and Environment School of EnvironmentHarbin Institute of TechnologyHarbin 150090China Department of Civil and Environmental engineering William&Cloy Codiga Resource Recovery CenterStanford UniversityStanfordCA 94305USA Plasticentropy rue Thiers 28Reims 51100France Department of Entomology and Department of Osteopathic Medical Specialties Michigan State UniversityEast LansingMI 48824USA School of Environmental Studies Cochin University of Science and TechnologyKochi 682022India Department of chemical engineering Pohang University of Science and TechnologyPohang 37673Republic of Korea School of Environmental science and engineering Tongji UniversityShanghai 200092China china Energy Conservation and Environmental Protection Group CECEP Talroad Technology Co.Ltd.Beijing 100096China School of Ecological and Environmental sciences East China Normal UniversityShanghai 200241China Research Institute for Frontier science Beihang UniversityBeijing 100191China School of Environment Tsinghua UniversityBeijing 100084China

Insects damaging and penetrating plastic packaged materials has been reported since the *** innovation breakthroughs of plastic biodegradation have been initiated since the discovery of biodegradation of plastics by Tenebrio molitor larvae in 2015 followed by Galleria mellonella in *** we review updated studies on the insect-mediated biodegradation of *** biodegradation by insect larvae,mainly by some species of darkling beetles(Tenebrionidae)and pyralid moths(Pyralidae)is currently a highly active and potentially transformative area of *** the past eight years,publications have increased explosively,including discoveries of the ability of different insect species to biodegrade plastics,biodegradation performance,and the contribution of host and microbiomes,impacts of polymer types and their physic-chemical properties,and responsible enzymes secreted by the host and gut *** date,almost all major plastics including polyethylene(PE),polypropylene(PP),polyvinyl chloride(PVC),polyethylene terephthalate(PET),polyurethane(PUR),and polystyrene(PS)can be biodegraded by *** and ten other insect species representing the Tenebrionidae and Pyralidae *** biodegradation processes are symbiotic reactions or performed by synergistic efforts of both host and gut-microbes to rapidly depolymerize and biodegrade plastics with hourly *** digestive ezymens and bioreagents screted by the insects play an essential role in plasatic biodegradation in certain species of Tenebrionidae and Pyralidae *** research on the insect itself,gut microbiomes,transcriptomes,proteomes and metabolomes has evaluated the mechanisms of plastic biodegradation in *** conclude this review by discussing future research perspectives on insect-mediated biodegradation of plastics.

关键词： Plastics Biodegradation Insects Gut microbiomes Enzymes

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Highly efficient solution-processed organic photovoltaics enabled by improving packing behavior of organic semiconductors

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science china Chemistry 2024年第3期67卷 890-897页

作者： Xinyue Cui Hongxiang Li hao Lu Yuqiang Liu Guangliu Ran Rui Liu Huarui Zhang Xueqing Ma Dawei Li Yi Lin Jifa Yu Wenkai Zhang lei Cai Yahui Liu Pei Cheng Andong Zhang Zaifei Ma Guanghao Lu Zhishan Bo College of Textiles and Clothing State Key Laboratory of Bio-fibers and Eco-textilesQingdao UniversityQingdao 266071China State Key Laboratory of Polymer Materials engineering College of Polymer Science and EngineeringSichuan UniversityChengdu 610065China Department of Physics and Applied Optics beijing Area Major Laboratory Center for Advanced Quantum StudiesBeijing Normal UniversityBeijing 100875China Shandong Province Key Laboratory of Medical Physics and Image Processing Technology School of Physics and ElectronicsShandong Normal UniversityJinan 250014China beijing Key Laboratory of Energy Conversion and Storage Materials College of ChemistryBeijing Normal UniversityBeijing 100875China Center for Advanced Low-Dimension Materials State Key Laboratory for Modification of Chemical Fibers and Polymer MaterialsCollege of Materials Science and EngineeringDonghua UniversityShanghai 201620China Frontier Institute of science and Technology Xi'an Jiaotong UniversityXi'an 710054China

Solution processability is a unique property of organic semiconductors. The compact and regular π-π stacking between molecules is paramount in the performance of organic optoelectronic devices. However, it is still a challenge to improve their stacking quality without sacrificing the solution-processability from the aspect of materials design. Here, delicately engineered additives are presented to promote the formation of ordered aggregation of conjugated molecules by regulating their nucleation and growth dynamics. Intriguingly, the long-chain BTP-eC9-4F molecules can realize ordered aggregation comparable to short-chain ones without sacrificing processability. The domain size of BTP-eC9-4F aggregation is enlarged from 24.2 to 32.2 nm in blend *** exciton diffusion and charge transport become faster, contributing to the suppression of recombination losses. As a result, a power conversion efficiency of 19.2% is achieved in D18:BTP-eC9-4F based organic photovoltaics. Our findings demonstrate a facile strategy to improve the packing quality of solution-processed organic semiconductors for high-efficiency photovoltaics and beyond photovoltaics.

关键词： organic semiconductor organic photovoltaic charge transport solution processability

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Two-dimensional materials for future information technology: status and prospects

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science china(Information sciences) 2024年第6期67卷 1-147页

作者： hao QIU Zhihao YU Tiange Zhao Qi ZHANG Mingsheng XU Peifeng LI Taotao LI Wenzhong BAO Yang CHAI Shula CHEN Yiqi CHEN Hui-Ming CHENG Daoxin DAI Zengfeng DI Zhuo DONG Xidong DUAN Yuhan feng Yu FU Jingshu GUO Pengwen GUO Yue hao Jun HE Xiao HE Jingyi HU Weida HU Zehua HU Xinyue HUANG Ziyang HUANG Ali IMRAN Ziqiang KONG Jia LI Qian LI Weisheng LI lei LIAO Bilu LIU Can LIU Chunsen LIU Guanyu LIU Kaihui LIU Liwei LIU Sheng LIU Yuan LIU Donglin LU Likuan MA feng MIAO Zhenhua NI Jing NING Anlian PAN Tian-Ling REN haowen SHU Litao SUN Yue SUN Quanyang TAO Zi-Ao TIAN Dong WANG hao WANG haomin WANG Jialong WANG Junyong WANG Wenhui WANG Xingjun WANG Yeliang WANG Yuwei WANG Zhenyu WANG Yao WE Department of Applied Physics The Hong Kong Polytechnic University Key Laboratory for Micro-Nano Physics and Technology of Hunan Province College of Materials Science and EngineeringHunan University College of Integrated Circuits Zhejiang University Shenzhen Geim Graphene Center Shenzhen Key Laboratory of Layered Materials for Value-Added ApplicationsTsinghua-Berkeley Shenzhen Institute & Institute of Materials ResearchTsinghua Shenzhen International Graduate SchoolTsinghua University State Key Laboratory of Extreme Photonics and Instrumentation College of Optical Science and EngineeringInternational Research Center for Advanced PhotonicsZijingang CampusZhejiang University National Key Laboratory of Materials for Integrated Circuits Shanghai Institute of Microsystem and Information TechnologyChinese Academy of Sciences CAS Key Laboratory of Nanophotonic Materials and Devices & Key Laboratory of Nanodevices and Applications i-LabSuzhou Institute of Nano-Tech and Nano-Bionics (SINANO)Chinese Academy of Sciences College of Chemistry and chemical engineering Hunan University Key Laboratory of Quantum State Construction and Manipulation (Ministry of Education) Department of PhysicsRenmin University of China School of Integrated Circuits Beijing National Research Center for Information Science and Technology (BNRist)Tsinghua University School of Electronic science and engineering Nanjing University The State Key Discipline Laboratory of Wide Band Gap Semiconductor Technology Shaanxi Joint Key Laboratory of GrapheneSchool of MicroelectronicsXidian University Key Laboratory of Artificial Micro- and Nano-Structures of Ministry of Education School of Physics and TechnologyWuhan University School of Integrated Circuits Huazhong University of Science and Technology Center for Nanochemistry (CNC) Beijing Science and Engineering Center for NanocarbonsBeijing National Laboratory for Molecular SciencesCollege of Chemistry and Molecular EngineeringPeking University State Key Laboratory for Artificial Microstruct

Over the past 70 years, the semiconductor industry has undergone transformative changes,largely driven by the miniaturization of devices and the integration of innovative structures and materials. Two-dimensional(2D) materials like transition metal dichalcogenides(TMDs) and graphene are pivotal in overcoming the limitations of silicon-based technologies, offering innovative approaches in transistor design and functionality, enabling atomic-thin channel transistors and monolithic 3D integration. We review the important progress in the application of 2D materials in future information technology, focusing in particular on microelectronics and optoelectronics. We comprehensively summarize the key advancements across material production, characterization metrology, electronic devices, optoelectronic devices, and heterogeneous integration on silicon. A strategic roadmap and key challenges for the transition of 2D materials from basic research to industrial development are outlined. To facilitate such a transition, key technologies and tools dedicated to 2D materials must be developed to meet industrial standards, and the employment of AI in material growth, characterizations, and circuit design will be essential. It is time for academia to actively engage with industry to drive the next 10 years of 2D material research.

关键词： two-dimensional (2D) materials information technology production technology standardization of characterization microelectronicdevices optoelectronic devices multi-functional integration

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秸秆添加对长期施肥旱地红壤N_(2)O和CO_(2)排放的影响

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环境科学 2024年第6期45卷 3716-3724页

作者：涂昊泽林杉王军胡荣桂肖恒斌邬磊华中农业大学资源与环境学院农业农村部长江中下游耕地保育重点实验室武汉430070 中国农业科学院农业资源与农业区划研究所北方干旱半干旱耕地高效利用全国重点实验室北京100081

秸秆还田作为农田土壤培肥的一种重要措施,显著影响N_(2)O和CO_(2)等温室气体排放.为探明长期施肥土壤N_(2)O和CO_(2)排放对秸秆添加的响应规律及关键影响因素,采集对照(CK,不施肥)、当地推荐化肥施用量(F)、200%当地推荐化肥施用量(2F... 详细信息

秸秆还田作为农田土壤培肥的一种重要措施,显著影响N_(2)O和CO_(2)等温室气体排放.为探明长期施肥土壤N_(2)O和CO_(2)排放对秸秆添加的响应规律及关键影响因素,采集对照(CK,不施肥)、当地推荐化肥施用量(F)、200%当地推荐化肥施用量(2F)、猪粪(M)和化肥配施猪粪(FM)这5种长期施肥(30 a)处理的旱地红壤,分别设置添加秸秆和不添加秸秆处理,在恒温恒湿条件下培养(65%田间持水量,25℃)20 d.结果表明,施肥显著促进了N_(2)O排放.相较不施肥处理[(22.05±2.09)μg·kg^(-1),以N计,下同],施化肥处理N_(2)O累计排放量显著增加了119%~195%[F和2F处理分别为(48.38±20.81)μg·kg^(-1)和(65.13±12.55)μg·kg^(-1)],施粪肥处理N_(2)O累计排放量显著增加了275%~399%[M和FM处理分别为(82.72±12.73)μg·kg^(-1)和(1101.99±425.71)μg·kg^(-1)].土壤硝态氮(NO_(3)^(-)-N)、可溶性有机碳(DOC)和可溶性总氮(DTN)是影响不同施肥处理N_(2)O排放的主要因素.相较未添加秸秆,添加秸秆对CK、F和FM处理的N_(2)O累计排放无显著影响,显著增加了2F(345%)和M处理(247%)的N_(2)O累计排放.秸秆添加通过增加DOC和消耗DTN从而影响N_(2)O排放.施肥显著促进了CO_(2)排放.相较不施肥处理,施粪肥处理CO_(2)累计排放量显著增加了120%~130%[M和FM处理累计排放量(以C计,下同),分别为(122.11±4.3)mg·kg^(-1)和(116.47±4.55)mg·kg^(-1)],2F处理CO_(2)累计排放量显著增加了28%[(65.13±12.55)mg·kg^(-1)].微生物量碳(MBC)、DOC和DTN是影响不同施肥处理CO_(2)排放的主要因素.相较未添加秸秆,添加秸秆条件下CO_(2)累计排放量显著增加了660%~1132%.秸秆添加后DOC和MBC含量显著提高,促进了CO_(2)排放.综上,秸秆添加通过增加土壤DTN消耗和DOC含量显著促进施肥处理的N_(2)O和CO_(2)排放.在施用粪肥的旱地红壤中应合理考虑秸秆还田,以平衡肥力提升与温室气体排放的综合效益.

关键词：长期施肥土壤秸秆添加 N_(2)O CO_(2) 土壤化学性质偏最小二乘法路径分析模型(PLS-PM)

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Functional Peptides from One-bead One-compound High-throughput Screening Technique

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chemical Research in Chinese Universities 2023年第1期39卷 83-91页

作者： YAN Yaqiong WANG lei WANG hao CAS Center for Excellence in Nanoscience CAS Key Laboratory for Biomedical Effects of Nanomaterials and NanosafetyNational Center for Nanoscience and Technology(NCNST)Beijing100190P.R.China Center of Materials science and Optoelectronics engineering University of Chinese Academy of SciencesBeijing100049P.R.China

Combinatorial chemistry provides a cost-effective method for the rapid discovery of new functional ***-bead one-compound(OBOC)high-throughput screening technique offers a lot of structurally diverse peptides to be rapidly synthesized and screened for binding to a target of *** OBOC peptide library screening involves three main steps:library construction,positive beads separation,and peptide *** review mainly summarizes some special technique tips during functional peptide screening and potential future directions of the OBOC high-throughput screening technique.

关键词： Combinatorial chemistry One-bead one-compound(OBOC) Cyclic peptide Peptide screening Self-assembly

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Global Fujita-Kato's Type Solutions and Long-time Behavior for the Multidimensional Chemotaxis Model

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Acta Mathematica Sinica,English Series 2022年第2期38卷 311-330页

作者： Qiong lei CHEN Xiao Nan hao Jing Yue LI Institute of Applied Physics and Computational Mathematics Beijing 100088P.R.China School of Mathematical sciences Peking UniversityBeijing 100871P.R.China

We establish the global well-posedness for the multidimensional chemotaxis model with some classes of large initial data,especially the case when the rate of variation of ln v0(v0 is the chemical concentration)contains high oscillation and the initial density near the equilibrium is allowed to have large oscillation in ***,we show the optimal time-decay rates of the strong solutions under an additional perturbation assumption,which include specially the situations of d=2,3 and improve the previous time-decay *** method mainly relies on the introduce of the effective velocity and the application of the localization in Fourier spaces.

关键词： Critical Besov spaces chemotaxis model global well-posedness optimal time-decay rates

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A review of whole-process control of industrial volatile organic compounds in china

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Journal of Environmental sciences 2023年第1期123卷 127-139页

作者： Hailin Wang Shumei Sun lei Nie Zhongshen Zhang Wenpeng Li Zhengping hao beijing Key Laboratory for Urban Atmospheric VOCs Pollution Control and Technology Application Beijing Municipal Research Institute of Environmental ProtectionBeijing 100037China College of Resources Environment and Tourism Capital Normal UniversityBeijing 100048China National engineering Laboratory for VOCs Pollution Control Material&Technology Research Center for Environmental Material and Pollution Control TechnologyUniversity of Chinese Academy of SciencesBeijing 101408China

Volatile organic compounds(VOCs)play an important role in the formation of ground-level ozone and secondary organic aerosol(SOA),and they have been key issues in current air pollution prevention and control in *** attention has been paid to industrial activities due to their large and relatively complex VOCs *** present research aims to provide a comprehensive review on whole-process control of industrial VOCs,which mainly includes source reduction,collection enhancement and end-pipe *** VOCs materials including water-borne ones are the keys to source substitution in industries related to coating and solvent usage,leak detection and repair(LDAR)should be regarded as an efficient means of source reduction in refining,petrochemical and other chemical *** types of VOCs collection methods such as gas-collecting hoods,airtight partitions and others are discussed,and airtight collection at negative pressure yields the best collection *** end-pipe treatments like UV oxidation,low-temperature plasma,activated carbon adsorption,combustion,biodegradation,and adsorption-combustion are discussed in ***,several recommendations are made for future advanced treatment and policy development in industrial VOCs emission control.

关键词： Volatile organic compounds Materials substitution Collection enhancement End-pipe treatments

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