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Engineering Single Atom Catalysts for Flow Production:From Catalyst Design to Reactor Understandings

Accounts of Materials Research 2023年第1期4卷 27-41页

作者： zhongxin chen Jia Liu Kian Ping Loh Department of Chemistry National University of SingaporeSingapore 117543Singapore

CONSPECTUS:In heterogeneous catalysis,the long-standing challenge isto achieve extremely high activity and chemoselectivity in liquid-phaseorganic transformations comparable to that of homogeneous or enzymaticprocesses.Single-atom catalysts(SACs)with atomically precise coordinationare developed with the objectives to mimic the homogeneous pathwaysbut face stability issues due to metal leaching or clustering.Additionally,thepractical application of SACs in chemical production is hampered by thelack of standard preparation protocols and low conversion using laboratorybatch reactors.This Account focuses on our recent studies in both catalyst design andreactor-level engineering for the flow synthesis of fine chemicals via SACs.At the catalyst and reaction level,we will discuss the intrinsic mechanismthat controls reactivity and chemoselectivity in the SAC-catalyzed processand highlight examples where SACs outperform other catalytic approaches.Specifically,we reported the SAC-mediated preparationand late-stage functionalization of pharmaceutical drugs,including lonidamine,Tamiflu,cavosonstat,indomethacin,and many othersby chemoselective transformations in a sequential or multicomponent manner.The ability of ultrahigh loading SACs in providing amultisite pathway for organic transformations involving two or more reactants is highlighted and contrasted with the single-sitepathway in conventional SACs.Molecular-level understanding on the dynamic catalytic cycle obtained using operando X-rayabsorption spectroscopies provides guidance for the design of more effective and leach resistant SACs.This also calls for thetransformation of laboratory powder-based catalysts into industrially viable monolithic catalysts via formulation to further enhancethe leach resistance.At the reactor level,we will highlight the importance of continuous-flow techniques in maximizing productivityand simplifying process transfer from laboratory to commercial production.Particularly,we discuss the use of fuel cell-type flowstacks for quantitative pr

关键词： catalyst overcome kinetics

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Design of Photothermal Covalent Organic Frameworks by Radical Immobilization

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CCS Chemistry 2022年第8期4卷 2842-2853页

作者： Xiaohui Tang zhongxin chen Qing Xu Yan Su Hong Xu Satoshi Horike Huanhuan Zhang Yuan Li cheng Gu State Key Laboratory of Luminescent Materials and Devices Institute of Polymer Optoelectronic Materials and DevicesSouth China University of TechnologyGuangzhou 510640 CAS Key Laboratory of Low-Carbon Conversion Science and Engineering Shanghai Advanced Research Institute(SARI)Chinese Academy of Sciences(CAS)Shanghai 201210 Institute of Nuclear and New Energy Technology Tsinghua UniversityBeijing 100084 Institute for Integrated Cell-Material Sciences Institute for Advanced StudyKyoto UniversityYoshidaSakyo-kuKyoto 606-8501 Guangdong Provincial Key Laboratory of Luminescence from Molecular Aggregates South China University of TechnologyGuangzhou 510640

Covalent organic frameworks(COFs)characterized by structural diversity,face-to-face stacking and open channels exhibit unique advantages as photothermal materials but have rarely been applied in solar-driven water evaporation due to complicated framework design,tedious synthesis,and low solar-to-vapor efficiency.Herein,we report a materials design strategy to produce efficient and robust photothermal COF by anchoring nonemissive radicals to the pore surface by a[2+2]cycloaddition–retroelectrocyclization reaction.

关键词： covalent organic frameworks radicals photothermal conversion water evaporation

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Improving a PenmanMonteith evapotranspiration model by incorporating soil moisture control on soil evaporation in semiarid areas

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International Journal of Digital Earth 2013年第S1期6卷 134-156页

作者： Liang Sun Shunlin Liang Wenping Yuan zhongxin chen State Key Laboratory of Remote Sensing Science Jointly Sponsored by Beijing Normal University and Institute of Remote Sensing ApplicationsChinese Academy of ScienceBeijingChina College of Global Change and Earth System Science Beijing Normal UniversityBeijingChina Department of Geography University of MarylandCollege ParkMDUSA Institute of Agricultural Resources and Regional Planning Chinese Academy of Agricultural SciencesBeijingChina

PenmanMonteith(PM)theory has been successfully applied to calculate land surface evapotranspiration(ET)for regional and global scales.However,soil surface resistance,related to soil moisture,is always difficult to determine over a large region,especially in arid or semiarid areas.In this study,we developed an ET estimation algorithm by incorporating soil moisture control,a soil moisture index(SMI)derived from the surface temperature and vegetation index space.We denoted this ET algorithm as the PM-SMI.The PM-SMI algorithm was compared with several other algorithms that calculated soil evaporation using relative humidity,and validated with Bowen ratio measurements at seven sites in the Southern Great Plain(SGP)that were covered by grassland and cropland with low vegetation cover,as well as at three eddy covariance sites from AmeriFlux covered by forest with high vegetation cover.The results show that in comparison with the other methods examined,the PM-SMI algorithm significantly improved the daily ET estimates at SGP sites with a root mean square error(RMSE)of 0.91 mm/d,bias of 0.33 mm/d,and R^(2) of 0.77.For three forest sites,the PM-SMI ET estimates are closer to the ET measurements during the non-growing season when compared with the other three algorithms.At all the 10 validation sites,the PMSMI algorithm performed the best.PM-SMI 8-day ET estimates were also compared with MODIS 8-day ET products(MOD16A2),and the latter showed negligible bias at SGP sites.In contrast,most of the PM-SMI 8-day ET estimates are around the 1:1 line.

关键词： ET PenmanMonteith soil moisture MODIS

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Rational synthesis of carbon shell coated polyaniline/ MoS2 monolayer composites for high-performance supercapacitors

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Nano Research 2016年第4期9卷 951-962页

作者： Chao Yang zhongxin chen Imran Shakir Yuxi Xu Hongbin Lu State Key Laboratory of Molecular Engineering of Polymers Department of Macromolecular Science Collaborative Innovation Center of Polymers and Polymer Composite Materials Fudan University Shanghai 200433 China Sustainable Energy Technologies (SET) center College of Engineering King Saud University PO-BOX 800 Riyadh 11421 Kingdom of Saudi Arabia

Conducting polymers generally show high specific capacitance but suffer from poor rate capability and rapid capacitance decary which greatly limits their practical applications in supercapacitor electrodes. To this end, many studies have focused on improving the overall capacitive performance by synthesizing nanostructured conducting polymers or by depositing a range of coatings to increase the active surface area exposed to the electrolyte and enhance the charge transport efficiency and structural stability. Despite this, simultaneously achieving high specific capacitance, good rate performance, and long cycle life remains a considerable challenge. Among the various two-dimensional （2D） layered materials, octahedral （1T） phase molybdenum disulfide （MoS2） nano- sheets have high electrical conductivity, large specific surface areas, and unique surface chemical characteristics, making them an interesting substrate for the controlled growth of nanostructured conducting polymers. This paper reports the rational synthesis of carbon shell-coated polyaniline （PANI） grown on 1T MoS2 monolayers （MoS2/PANI@C）. The composite electrode comprised of MoS2/ PANI@C with a -3 nm carbon shell exhibited a remarkable specific capacitance of up to 678 F-g-1 （1 mV.s-1）, superior capacity retention of 80% after 10,000 cycles and good rate performance （81% at 10 mV.s-1） due to the multiple synergic effects between the PANI nanostructure and 1T MoS2 substrates as well as protection by the uniform thin carbon shell. These properties are comparable to the best overall capacitive performance achieved for conducting polymers-based supercapacitor electrodes reported thus far.

关键词： supercapadtor,polyaniline,molybdenum disulfide,carbon shell,cycle stability

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Near-infrared organic photoelectric materials for lightharvesting systems: Organic photovoltaics and organic photodiodes

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InfoMat 2020年第1期2卷 57-91页

作者： Boming Xie zhongxin chen Lei Ying Fei Huang Yong Cao Institute of Polymer Optoelectronic Materials and Devices State Key Laboratory of Luminescent Materials and DevicesSouth China University of TechnologyGuangzhouPR China

The inherent advantages of organic optoelectronic materials endow lightharvesting systems,including organic photovoltaics(OPVs)and organic photodiodes(OPDs),with multiple advantages,such as low-cost manufacturing,light weight,flexibility,and applicability to large-area fabrication,make them promising competitors with their inorganic counterparts.Among them,nearinfrared(NIR)organic optoelectronic materials occupy a special position and have become the subject of extensive research in both academia and industry.The introduction of NIR materials into OPVs extends the absorption spectrum range,thereby enhancing the photon-harvesting ability of the devices,due to which they have been widely used for the construction of semitransparent solar cells with single-junction or tandem architectures.NIR photodiodes have tremendous potential in industrial,military,and scientific applications,such as remote control of smart electronic devices,chemical/biological sensing,environmental monitoring,optical communication,and so forth.These practical and potential applications have stimulated the development of NIR photoelectric materials,which in turn has given impetus to innovation in light-harvesting systems.In this review,we summarize the common molecular design strategies of NIR photoelectric materials and enumerate their applications in OPVs and OPDs.

关键词： near infrared organic optoelectronic materials organic photodiodes organic photovoltaics

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Molecular design towards two-dimensional electron acceptors for efficient non-fullerene solar cells

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Journal of Energy Chemistry 2020年第12期29卷 190-198页

作者： Yan Liu Zixian Liu Zhicheng Hu Yuanying Liang Zhenfeng Wang zhongxin chen Fei Huang Yong Cao Institute of Polymer Optoelectronic Materials and Devices State Key Laboratory of Luminescent Materials and DevicesSouth China University of TechnologyGuangzhou 510640GuangdongChina

Non-fullerene polymer solar cells(NF-PSCs) have gained wide attention recently. Molecular design of non-fullerene electron acceptors effectively promotes the photovoltaic performance of NF-PSCs. However,molecular electron acceptors with 2-dimensional(2 D) configuration and conjugation are seldom reported.Herein, we designed and synthesized a series of novel 2 D electron acceptors for efficient NF-PSCs. With rational optimization on the conjugated moieties in both vertical and horizontal direction, these 2 D electron acceptors showed appealing properties, such as good planarity, full-spectrum absorption, high absorption extinction coefficient, and proper blend morphology with donor polymer. A high PCE of 9.76%was achieved for photovoltaic devices with PBDB-T as the donor and these 2 D electron acceptors. It was also found the charge transfer between the conjugated moieties in two directions of these 2 D molecules contributes to the utilization of absorbed photos, resulting in an exceptional EQE of 87% at 730 nm. This work presents rational design guidelines of 2 D electron acceptors, which showed great promise to achieve high-performance non-fullerene polymer solar cells.

关键词： Two-dimensional molecules Perylene diimide Electron acceptors Molecular design Non-fullerene solar cells

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浅谈对广元市山地海绵城市建设的若干思考

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建设科技 2024年第2期 68-70页

作者：陈中新广元城发零八壹勘察设计集团有限公司广元628000

海绵城市的建设工作在平原地带已经有了丰富的实践经验,各个地区也制订了相关图集和规范,但在山地海绵城市建设还缺少相关经验。四川省的一众城市都是山地、丘陵为主的地貌。广元市有着山地河谷类型为主的主城区地势,借由建设海绵城市... 详细信息

海绵城市的建设工作在平原地带已经有了丰富的实践经验,各个地区也制订了相关图集和规范,但在山地海绵城市建设还缺少相关经验。四川省的一众城市都是山地、丘陵为主的地貌。广元市有着山地河谷类型为主的主城区地势,借由建设海绵城市示范城市为契机打造山地河谷型海绵城市。本文通过梳山理水、结合山地地势,探讨适用于山地城市的径流控制措施,强调海绵城市建设与城市更新、城市公园建设、建设生态护岸等行动结合,从而为全国山地海绵城市建设工作提供参考。

关键词：山地海绵梳山理水径流控制低影响开发设施城市更新

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Ultrahigh Loading Copper Single Atom Catalyst for Palladium-free Wacker Oxidation

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Chemical Research in Chinese Universities 2022年第5期38卷 1239-1242页

作者： SONG Jingting LIU Jia LOH Kian Ping chen zhongxin Department of Chemistry National University of SingaporeSingapore 117543Singapore Joint School of National University of Singapore and Tianjin University International Campus of Tianjin UniversityFuzhou 350207P.R.China

Wacker oxidation is an industry-adopted process to transform olefins into value-added epoxides and carbonyls.However,traditional Wacker oxidation involves the use of homogeneous palladium and copper catalysts for the olefin addition and reductive elimination.Here,we demonstrated an ultrahigh loading Cu single atom catalyst(14%Cu,mass fraction)for the palladium-free Wacker oxidation of 4-vinylanisole into the corresponding ketone with N-methylhydroxylamine hydrochloride as an additive under mild conditions.Mechanistic studies by ^(18)O and deuterium isotope labelling revealed a hydrogen shift mechanism in this palladium-free process using N-methylhydroxylamine hydrochloride as the oxygen source.The reaction scope can be further extended to Kucherov oxidation.Our study paves the way to replace noble metal catalysts in the traditional homogeneous processes with single atom catalysts.

关键词： Single atom catalyst Wacker oxidation Ultrahigh loading High valued chemical Organic catalysis

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系统性红斑狼疮患者外周血CD19^(+)CD25^(+)Breg比例和细胞表面PD-1和PD-L1的表达及其与临床指标的相关性

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细胞与分子免疫学杂志 2024年第2期40卷 148-157页

作者：谢卓贝代丽何豪华洪登校王元元徐文艳陈中新李柏青谢长好蚌埠医科大学第一附属医院风湿免疫科安徽蚌埠23300 徐州医科大学第二附属医院老年科江苏徐州221000 蚌埠医科大学组织与胚胎学教研室安徽蚌埠233000 蚌埠医科大学第一附属医院检验科安徽蚌埠233000 慢性疾病免疫学基础与临床安徽省重点实验室安徽蚌埠233000 炎症相关性疾病基础与转化研究安徽省重点实验室安徽蚌埠233000

目的研究程序性死亡蛋白1(PD-1)与其配体PD-L1在系统性红斑狼疮(SLE)患者外周血CD19^(+)CD25^(+)调节性B细胞(Breg)的表达及临床意义。方法收集50例SLE患者和41例健康人(HC)外周血标本,采用流式细胞仪检测外周血中CD19^(+)CD25^(+)Bre... 详细信息

目的研究程序性死亡蛋白1(PD-1)与其配体PD-L1在系统性红斑狼疮(SLE)患者外周血CD19^(+)CD25^(+)调节性B细胞(Breg)的表达及临床意义。方法收集50例SLE患者和41例健康人(HC)外周血标本,采用流式细胞仪检测外周血中CD19^(+)CD25^(+)Breg的比例,以及CD19^(+)CD25^(+)Breg的PD-1、PD-L1表达,同时采集患者的临床表现和实验室指标等临床信息。使用免疫磁珠分选CD4^(+)T细胞与CD19^(+)B细胞,体外细胞共培养,检测Breg的分化。结果SLE患者活动组外周血中CD19^(+)CD25^(+)Breg比例低于HC,CD25^(+)B细胞PD-1、PD-L1的表达高于HC;SLE患者有胸腔积液、关节炎、C反应蛋白(CRP)上升的患者Breg频率高于对应阴性组;SLE患者有IgM下降、抗核糖核蛋白(RNP)抗体阳性的患者Breg频率低于对应阴性组;SLE患者有感染、发热、关节炎、IgA上升的患者CD19^(+)CD25^(+)PD-1^(+)细胞频率高于对应阴性组;SLE患者有感染、发热、IgA上升的患者CD19^(+)CD25^(+)PD-L1^(+)细胞频率高于对应阴性组;活化的CD4^(+)T细胞有利于CD19^(+)B细胞表面CD25的表达。结论SLE患者外周血中CD19^(+)CD25^(+)Breg降低,但细胞表面PD-1与PD-L1的表达增加,并且与相关临床表现及实验室参数存在一定的关系。活化的CD4^(+)T细胞促进Breg的分化。

关键词：系统性红斑狼疮(SLE) CD19^(+)CD25^(+)调节性B细胞(Breg) 程序性死亡蛋白1(PD-1) 程序性死亡蛋白1配体1(PD-L1)

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AN AGENT-BASED POPULATION MODEL FOR CHINA

AN AGENT-BASED POPULATION MODEL FOR CHINA

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Computer and Computing Technologies in Agriculture——First IFIP TC 12 International Conference(CCTA2007) Volume I

作者： zhongxin chen Einar Holm Huajun Tang Kalle Mkil Wenjuan Li Shenghe Liu Key Laboratory of Resource Remote Sensing and Digital Agriculture Ministry of Agriculture Institute of Agriculture Resources®ional Planning Chinese Academy of Agricultural Sciences Kiruna Spatial Modelling Centre Umea University Institute of Geographical Science&Natural Resources Research

Human is a crucial factor responsible for local and large scale environmental change and is a key factor in rural management.Accurate simulating and predicting population change and its spatial distribution is of great interests to environmental scientists as well as social scientists.In this paper,we introduced the development of a spatial-explicit agent-based population model for China based on a prototype from SVERIGE model.The model was used to predict the population in China.The validation result shows that agent-based model performances well in population prediction in China.

关键词： Agent-Based Model SVERIGE Population Prediction China

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