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Room-temperature and atmospheric-pressure hydrogenation of lignin-derived phenol to KA oil by Pt/NiO@MOFs

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Nano Research 2024年第8期17卷 7053-7060页

作者： Fengbin Zheng Kun Wang Yifei Ren Bohua Wang Wenxing Chen caoyu yang Shengxian Shao Yinglong Wang Zhiyong Tang Guodong Li College of Chemical Engineering Qingdao University of Science and TechnologyQingdao 266042China CAS Key Laboratory of Nanosystem and Hierarchical Fabrication CAS Center for Excellence in NanoscienceNational Center for Nanoscience and TechnologyBeijing 100190China School of Materials Science and Engineering Beijing Institute of TechnologyBeijing 100181China School of Nanoscience and Technology University of Chinese Academy of SciencesBeijing 100049China

Hydrogenation of lignin-derived phenol to KA oil(the mixture of cyclohexanone(K)and cyclohexanol(A))is attractive yet challenging in the sustainable upgrading of biomass derivatives under mild *** supported metal catalysts have been widely studied but the active components on supports often exhibit low recyclability due to their instability under experimental *** we show fabricating ultrasmall Pt/NiO in the pores of chromium terephthalate MIL-101 as catalysts for hydrogenation of ***,Pt/NiO@MIL-101 achieves catalytic phenol hydrogenation to KA oils of tunable K/A ratios and good reusability under room temperature and atmospheric hydrogen pressure,superior to contrast Pt@MIL-101 and Pt/NiO *** excellent performance mainly originates from the effective adsorption and activation of phenol by coordinatively unsaturated Cr sites and H2 activation on ultrasmall Pt/NiO as well as its effective spillover to the adsorbed phenol over Cr sites for hydrogenation ***,such catalyst also displays the excellent performances for hydrogenation of phenol’s derivatives under mild conditions.

关键词： ultrasmall Pt/NiO MIL-101 phenol hydrogenation KA oil

Coordinating Zirconium Nodes in Metal-Organic Framework with Trifluoroacetic Acid for Enhanced Lewis Acid Catalysis

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Chemical Research in Chinese Universities 2022年第5期38卷 1301-1307页

作者： WANG Wenyang LIU Hanlin yang caoyu FAN Ting CUI Chengqian LU Xiaoquan TANG Zhiyong LI Guodong Department of Chemistry School of ScienceTianjin UniversityTianjin 300072P.R.China CAS Key Laboratory of Nanosystem and Hierarchical Fabrication CAS Center for Excellence in NanoscienceNational Center for Nanoscience and TechnologyBeijing 100190P.R.China School of Nanoscience and Technology University of Chinese Academy of SciencesBeijing 100049P.R.China Key Laboratory of Bioelectrochemistry&Environmental Analysis of Gansu Province College of Chemistry&Chemical EngineeringNorthwest Normal UniversityLanzhou 730070P.R.China

Regulating Lewis acid sites with well-defined electronic state and steric environment is still challenging for achieving high catalytic *** we show coordinating zirconium nodes in the typical metal-organic framework known as MOF-545 with the monocarboxylate modulators including trifluoroacetic acid(TFA)or benzoic acid(BA)over meso-tetra(4-carboxyphenyl)-porphine(H_(2)TCPP),denoted as MOF-545-TFA or ***,MOF-545-TFA shows the significantly enhanced performance for the catalytic ring-opening reaction of various epoxides with alcohols and good recyclability at 40°C in respect with MOF-545-BA and ZrO_(2).This mainly originates from the stronger Lewis acidity and more active zirconium sites induced by the electron-withdrawing TFA,resulting in the increased ability for activation of *** modulation approach is promising for enlarging the toolbox to extend the MOFs-based Lewis acid catalysis.

关键词： Metal-organic framework Active zirconium site Trifluoroacetic acid Epoxide ring-opening Modulator effect

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绿色氧化剂催化苯胺氧化偶联反应的研究进展

高等学校化学学报 2024年第8期45卷 21-34页

作者：班志勇杨曹雨冯清殷国俊李国栋烟台大学化学化工学院烟台264005 中国科学院纳米系统与多级次制造重点实验室中国科学院纳米科学卓越创新中心国家纳米科学中心北京100190 中国科学院大学纳米科学与工程学院北京100049

偶氮苯和氧化偶氮苯类化合物在颜料、光学材料、荧光探针和光电器件等领域具有广泛的应用前景.目前,已发展了不同的催化剂和氧化剂用于苯胺氧化偶联制备偶氮苯及氧化偶氮苯类化合物,其中开发绿色环保的氧化体系一直是该研究领域的热点... 详细信息

偶氮苯和氧化偶氮苯类化合物在颜料、光学材料、荧光探针和光电器件等领域具有广泛的应用前景.目前,已发展了不同的催化剂和氧化剂用于苯胺氧化偶联制备偶氮苯及氧化偶氮苯类化合物,其中开发绿色环保的氧化体系一直是该研究领域的热点和难点问题.本文综合评述了分别以双氧水和氧气作为氧化剂时,催化苯胺选择性氧化制备偶氮苯及氧化偶氮苯类化合物的研究进展,同时探讨了苯胺氧化的机理,主要包括亚硝基苯中间体机理与自由基偶联机理.最后,总结了催化剂合成和催化机制方面存在的潜在问题和挑战,并对未来的研究方向进行了展望,从而为相关领域的发展提供借鉴.

关键词：苯胺选择性氧化偶联过氧化氢氧气偶氮类化合物

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调制金属有机框架节点拓扑构型用于促进苯胺高效催化氧化

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中国科学：化学 2022年第9期52卷 1712-1721页

作者：杨曹雨张钊阳赵文世唐智勇中国科学院纳米系统与多级次制造重点实验室中国科学院纳米卓越创新中心国家纳米科学中心北京100190 中国科学院大学纳米科学与技术学院北京100049 中国科学院大学材料科学与光电技术学院北京100049

金属有机框架所具有的拓扑构型丰富的可调控性是其独特于传统多孔材料的显著特征之一.通过简单易行的方式调控组成构建金属有机框架的节点构型从而改变其拓扑堆积方式,并研究其催化性能的变化,这有助于深入理解催化反应的构效关系并为... 详细信息

金属有机框架所具有的拓扑构型丰富的可调控性是其独特于传统多孔材料的显著特征之一.通过简单易行的方式调控组成构建金属有机框架的节点构型从而改变其拓扑堆积方式,并研究其催化性能的变化,这有助于深入理解催化反应的构效关系并为高效催化剂的开发提供指导.本文以高稳定性的Hf-UiO-66作为研究对象,合成了具有Hf_(12)节点的hcp构型UiO-66-hcp以及具有Hf_(6)节点的fcu构型UiO-66-fcu,其中hcp构型材料对苯胺选择性氧化至氧化偶氮苯的反应具有显著优于fcu构型材料的催化性能,且具有优异的催化稳定性及底物拓展性.因节点结构改变所致的拓扑构型差异显著影响了催化活性,且性能差异适用于多种底物及网状化学同系物UiO-67,其来源可能在于Hf_(12)及Hf_(6)节点中桥联μ-OH的空间环境差异.

关键词：金属有机框架拓扑构型调控节点催化选择性氧化

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锆基金属有机框架孔道工程用于毒剂催化降解

防化研究 2023年第3期2卷 1-18页

作者：杨曹雨高慧文唐智勇中国科学院纳米系统与多级次制造重点实验室中国科学院纳米科学卓越创新中心国家纳米科学中心中国科学院大学纳米科学与工程学院

开发对高毒性的毒剂具有高效催化降解能力的材料是化学安全领域的重要课题。锆基金属有机框架材料通常由锆-氧节点与各种有机连接体以配位相互作用连接形成，一方面具有大量可及的配位不饱和位点作为路易斯酸性位点，另一方面其锆-氧节... 详细信息

开发对高毒性的毒剂具有高效催化降解能力的材料是化学安全领域的重要课题。锆基金属有机框架材料通常由锆-氧节点与各种有机连接体以配位相互作用连接形成，一方面具有大量可及的配位不饱和位点作为路易斯酸性位点，另一方面其锆-氧节点和有机连接体多样的配位构型以及它们自身的可修饰性可产生丰富的孔道结构，有望通过合理设计成为针对毒剂降解的高效催化材料。本文系统总结了近期利用锆基金属有机框架孔道工程开发毒剂降解催化剂的研究进展，分别从锆-氧节点连接数调节、锆-氧节点功能化修饰、有机连接体功能化修饰以及多级次孔结构构建4个方面综述了孔道工程对于锆基金属有机框架降解毒剂催化性能的优化策略和调控机制，并讨论了该领域面临的挑战以及发展方向。

关键词：金属有机框架材料锆-氧节点孔道工程毒剂催化降解

APPLICATION OF A NEURAL NETWORK PREDICTOR/CONTROLLER TO DYNAMIC POSITIONING OF FLOATING STRUCTURES

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Journal of Hydrodynamics 2003年第1期15卷 31-44页

作者： LeeTzung-hang caoyu-song DepartmentofMechanicalEngineering TamkangUniversityTamsuiTaiwanChina SchoolofNavalArchitectureandMarineEngineering UniversityofNewOrleansNewOrleansLA70115

An on-line training functional-link neural network predictor/controller fordynamic positioning of water surface structures is described in this paper. The on-line trainingneural network predictor acquires the knowledge about the system using a small number of samples ofthe latest system status measured on board of the structure. The trained function-link neuralnetwork is used with an optimal controller to control the output of the system. The accuracy androbustness of the on-line training predictor are demonstrated through the numerical simulations oftwo ship maneuvers. The on-line training neural network predictor/controller is applied to thedynamic positioning (station-keeping) of a ship in a uniform current with and without externalenvironmental disturbances. The results of the numerical simulations are very satisfactory.

关键词： on-line training neural network predictor/ controller dynamicpositioning

Crystallization and Orientation Modulation Enable Highly Efficient Doctor-Bladed Perovskite Solar Cells

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Nano-Micro Letters 2023年第10期15卷 40-52页

作者： Jianhui Chang Erming Feng Hengyue Li yang Ding caoyu Long Yuanji Gao Yingguo yang Chenyi Yi Zijian Zheng Junliang yang Hunan Key Laboratory of Nanophotonics and Devices School of Physics and ElectronicsCentral South UniversityChangsha 410083HunanPeople’s Republic of China Shanghai Synchrotron Radiation Facility(SSRF) Shanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201204People’s Republic of China Department of Electrical Engineering Tsinghua UniversityBeijing 100084People’s Republic of China Department of Applied Biology and Chemical Technology Faculty of ScienceThe Hong Kong Polytechnic UniversityHong Kong 999077People’s Republic of China

With the rapid rise in perovskite solar cells(PSCs)performance,it is imperative to develop scalable fabrication techniques to accelerate potential ***,the power conversion efficiencies(PCEs)of PSCs fabricated via scalable two-step sequential deposition lag far behind the state-of-the-art spin-coated ***,the additive methylammonium chloride(MACl)is introduced to modulate the crystallization and orientation of a two-step sequential doctorbladed perovskite film in ambient *** can significantly improve perovskite film quality and increase grain size and crystallinity,thus decreasing trap density and suppressing nonradiative ***,MACl also promotes the preferred face-up orientation of the(100)plane of perovskite film,which is more conducive to the transport and collection of carriers,thereby significantly improving the fill *** a result,a champion PCE of 23.14%and excellent longterm stability are achieved for PSCs based on the structure of ITO/SnO_(2)/FA_(1-x)MA_xPb(I_(1-y)Br_y)_3/Spiro-OMeTAD/*** superior PCEs of 21.20%and 17.54%are achieved for 1.03 cm~2 PSC and 10.93 cm~2 mini-module,*** results represent substantial progress in large-scale two-step sequential deposition of high-performance PSCs for practical applications.

关键词： Crystallization regulation Orientation modulation Perovskite solar cells Doctor-blading Ambient condition

ESTIMATION OF ATMOSPHERIC INPUT OF MERCURY TO SOUTH LAKE AND JINGYUE POOL

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Chinese Geographical Science 2002年第1期12卷 86-89页

作者： FANGFeng－man caoyu－hong 等 ChangchunInstituteofGeography theChineseAcademyofSciencesChangchun130021P.R.China DepartmentofGeogaphy AnhuiNormalUniversityWuhu241000P.R.China

Taking South Lake and Jingyue Pool in Changchun as examples, we determined particulate Hg in ambient air and Hg concentration in precipitation. Results indicated that particulate Hg in air and Hg concentration in precipitation in both sites in nonheating period were lower than that in heating period, which is influenced by coal combustion. The annual particulate Hg concentrations of South Lake and Jingyue Pool were 0.254ng/m3 and 0.109ng/m3. The yearly average Hg concentrations in precipitation were 0.268μg/L(South Lake) and 0.108μg/L(Jingyue Pool). The higher particulate Hg concentration in air and Hg concentration in precipitation in South Lake than that of Jingyue Pool indicated that mercury deposition was influenced by anthropogenic sources(especially from coas combustion). Hg concentration in precipitation is related with particulate Hg in the atmosphere. Dry deposition fluxes were estimated by using dry deposition model on the base of particulate Hg concentrations in the atmosphere, they were 35.5μg/(m2.a) for South lake and 15.3μg/(m2.a) for Jingyue Pool. Combined with precipitation amount, wet deposition fluxes were estimated in these two sites, 152.2μg/(m2.a) for South Lake and 61.2μg/(m2.a) for Jingyue Pool. Atmospheric Hg deposition fluxes were 160.2g/a for South Lake and 328.62g/a for Jingyue Pool.

关键词： south lake jingyue pool atmospheric mercury precipitation depositionfluxes

Bridging buried interface enable 24.67%-efficiency doctor-bladed perovskite solar cells in ambient condition

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Nano Research 2024年第9期17卷 8068-8076页

作者： Jianhui Chang Erming Feng Xiangxiang Feng Hengyue Li yang Ding caoyu Long Siyuan Lu Haixia Zhu Wen Deng Jiayan Shi Yingguo yang Si Xiao Yongbo Yuan Junliang yang Hunan Key Laboratory for Super-microstructure and Ultrafast Process School of PhysicsCentral South UniversityChangsha 410083China Hunan Key Laboratory of Nanophotonics and Devices School of PhysicsCentral South UniversityChangsha 410083China Textile and Fashion Collage Hunan Institute of EngineeringXiangtan 411101China Shanghai Synchrotron Radiation Facility Shanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201204China State Key Laboratory of Powder Metallurgy Central South UniversityChangsha 410083China

Scalable deposition of high-efficiency perovskite solar cells(PSCs)is critical to accelerating their commercial ***,a significant number of defects are distributed at the buried interface of perovskite film fabricated by scalable deposition,exhibiting much negative influence on the efficiency and stability of ***,2-(N-morpholino)ethanesulfonic acid potassium salt(MESK)is incorporated as the bridging layer between the tin oxide(SnO_(2))electron transport layer(ETL)and the perovskite film deposited via scalable two-step doctor *** experiment and simulation results demonstrate that MESK can passivate the trap states of Sn suspension bonds,thereby enhancing the charge extraction and transport of the SnO_(2)***,the strong interaction with uncoordinated Pb ions can modulate the crystal growth and crystallographic orientation of perovskite film and passivate buried *** employing MESK interface bridging,PSCs fabricated via scalable doctor blading in ambient condition achieve a power conversion efficiency(PCE)of 24.67%,which is one of the highest PCEs for doctor-bladed PSCs,and PSC modules with an active area of 11.35 cm^(2)achieve a PCE of 19.45%.Furthermore,PSCs exhibit excellent long-term stability,and the unpackaged target device with a storage of 1680 h in ambient condition(25℃and humidity of 30%relative humidity(RH))can maintain more than 90%of the initial *** research provides a strategy for constructing a high-performance interface bridge between SnO_(2)ETL and perovskite film,and achieving efficient and stable large-area PSCs and modules fabricated via scalable doctor-blading process in ambient condition.

关键词： perovskite solar cells doctor blading buried interface defect passivation orientation regulation