检索结果-南通市图书馆

The proximity between hydroxyl and single atom determines the catalytic reactivity of Rh1/CeO_(2) single-atom catalysts

引用

Nano research 2024年第1期17卷 397-406页

作者： Danfeng Wu Shuyun Zhou Congcong Du Juan Li Jianyu Huang Hong-xia Shen Abhaya K.Datye Shan Jiang Jeffrey T.Miller Sen Lin Haifeng Xiong state key laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China state key laboratory of photocatalysis on energy and environment College of ChemistryFuzhou UniversityFuzhou 350002China Clean Nano energy center State Key Laboratory of Metastable Materials Science and TechnologyYanshan UniversityQinhuangdao 066004China College of Biology and Chemical engineering Jiaxing UniversityJiaxing 314000China Department of Chemical&Biological engineering University of New MexicoAlbuquerqueNM 8731-0001USA Davidson School of Chemical engineering Purdue UniversityWest LafayetteIN 47907-2100USA Innovation laboratory for Sciences and Technologies of energy materials of fujian Province(IKKEM) Xiamen 361102China fujian key laboratory of Rare-earth functional materials Fujian Shanhai Collaborative Innovation Center of Rare-earth Functional MaterialsLongyan 366300China

The local structure of the metal single-atom site is closely related to the catalytic activity of metal single-atom catalysts(SACs).However,constructing SACs with homogeneous metal active sites is a challenge due to the surface heterogeneity of the conventional support.Herein,we prepared two Rh1/CeO_(2)SACs(0.5Rh1/r-CeO_(2)and 0.5Rh1/c-CeO_(2),respectively)using two shaped CeO_(2)(rod and cube)exposing different facets,i.e.,CeO_(2)(111)and CeO_(2)(100).In CO oxidation reaction,the T100 of 0.5Rh1/r-CeO_(2)SACs is 120°C,while the T100 of 0.5Rh1/c-CeO_(2)SACs is as high as 200°C.Via in-situ CO diffuse reflectance infrared Fourier transform spectroscopy(CO-DRIFTS),we found that the proximity between OH group and Rh single atom on the plane surface plays an important role in the catalytic activity of Rh1/CeO_(2)SAC system in CO oxidation.The Rh single atom trapped at the CeO_(2)(111)crystal surface forms the Rh1(OH)adjacent species,which is not found on the CeO_(2)(100)crystal surface at room temperature.Furthermore,during CO oxidation,the OH group far from Rh single atom on the 0.5Rh1/c-CeO_(2)disappears and forms Rh1(OH)adjacent species when the temperature is above 150°C.The formation of Rh1(OH)adjacentCO intermediate in the reaction is pivotal for the excellent catalytic activity,which explains the difference in the catalytic activity of Rh single atoms on two different CeO_(2)planes.The formed Rh1(OH)adjacent-O-Ce structure exhibits good stability in the reducing atmosphere,maintaining the Rh atomic dispersion after CO oxidation even when pre-reduced at high temperature of 500°C.Density functional theory(DFT)calculations validate the unique activity and reaction path of the intermediate Rh1(OH)adjacentCO species formed.This work demonstrates that the proximity between metal single atom and hydroxyl can determine the formation of active intermediates to affect the catalytic performances in catalysis.

关键词： crystal plane Rh1/CeO_(2)single-atom catalyst proximity of Rh and hydroxyl coordination structure CO oxidation

来源：

维普期刊数据库评论

在线全文

维普期刊数据库

学校读者我要写书评

暂无评论

Temperature inversion enables superior stability for low-temperature Zn-ion batteries

引用

Journal of energy Chemistry 2024年第4期91卷 245-253页

作者： Fu-Da Yu Zhe-Jian Yi Rui-Yang Li Wei-Hao Lin Jie Chen Xiao-Yue Chen Yi-Ming Xie Ji-Huai Wu Zhang Lan Lan-Fang Que Bao-Sheng Liu Hao Luo Zhen-Bo Wang engineering research center of environment-Friendly functional materials Ministry of EducationInstitute of Materials Physical ChemistryHuaqiao UniversityXiamen 361021FujianChina b2 School of Electronic engineering Guangxi University of Science and TechnologyLiuzhou 545006GuangxiChina School of materials Science and engineering Xiamen University of TechnologyXiamen 361024FujianChina School of materials Science and engineering Zhengzhou UniversityZhengzhou 450001HenanChina MIIT key laboratory of Critical materials Technology for New energy Conversion and Storage State Key Laboratory of Space Power-SourcesSchool of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbin 150001HeilongjiangChina College of materials Science and engineering Shenzhen UniversityShenzhen 518071GuangdongChina

It is challenging for aqueous Zn-ion batteries(ZIBs)to achieve comparable low-temperature(low-T)performance due to the easy-frozen electrolyte and severe Zn dendrites.Herein,an aqueous electrolyte with a low freezing point and high ionic conductivity is proposed.Combined with molecular dynamics simulation and multi-scale interface analysis(time of flight secondary ion mass spectrometry threedimensional mapping and in-situ electrochemical impedance spectroscopy method),the temperature independence of the V_(2)O_(5)cathode and Zn anode is observed to be opposite.Surprisingly,dominated by the solvent structure of the designed electrolyte at low temperatures,vanadium dissolution/shuttle is significantly inhibited,and the zinc dendrites caused by this electrochemical crosstalk are greatly relieved,thus showing an abnormal temperature inversion effect.Through the disclosure and improvement of the above phenomena,the designed Zn||V_(2)O_(5)full cell delivers superior low-T performance,maintaining almost 99%capacity retention after 9500 cycles(working more than 2500 h)at-20°C.This work proposes a kind of electrolyte suitable for low-T ZIBs and reveals the inverse temperature dependence of the Zn anode,which might offer a novel perspective for the investigation of low-T aqueous battery systems.

关键词： Aqueous Zn-ion batteries Low-temperature performance Opposite temperature dependence Zndendrite growth Vanadium dissolution

来源：

维普期刊数据库

同方期刊数据库评论

在线全文

学校读者我要写书评

暂无评论

A novel hierarchical targeting and controllable smart nanoparticles for enhanced in situ nuclear photodynamic therapy

引用

Nano research 2022年第5期15卷 4212-4223页

作者： Gankun Yuan Qilu Wang Zifan You Xuening Chen Jinping Xue Xiao Jia Juanjuan Chen National&Local Joint Biomedical engineering research center on Photodynamic Technologies State Key Laboratory of Photocatalysis on Energy and EnvironmentCollege of ChemistryFuzhou UniversityFuzhou 350116China

Photodynamic therapy(PDT)is a promising and non-invasive treatment for various cancers.Although nuclear PDT has considerable therapeutic prospects,it is still hindered by the non-specific recognition of tumor tissues or the degradation of nuclear targeting cationic groups by enzymes in the blood.Herein,a hierarchical targeted and controlled release strategy is proposed by using folate-modified poly-β-cyclodextrin(poly-β-CD)as a nano-carrier for loading nuclear localization signals(NLSs)-conjugated photosensitizer PAP(PAP=pyropheophorbide a-PAAKRVKLD).Excitingly,the obtained FA-CD@PAP(FA=folic acid)and nanoparticles(NPs)can specifically recognize tumor cells overexpressing folate receptors(FR)to remarkedly enhance the intracellular accumulation.Furthermore,the encapsulated PAP can be released under acidic conditions to realize precise nuclear localization.The reactive oxygen species(ROS)generated by the intranuclear-accumulated PAP upon irradiation can oxidize and destroy DNA chains or DNA repair enzymes instantaneously,which can directly induce cell death.As a result,FA-CD@PAP NPs exhibit excellent tumor regression and negligible side effects.This work provides an intelligent nuclear-targeted delivery strategy for in situ nuclear PDT with extremely prominent efficacy and high biological safety.

关键词： photodynamic therapy hierarchical targeted nuclear localization signal poly-β-cyclodextrin nuclear-targeted

来源：

维普期刊数据库评论

在线全文

维普期刊数据库

学校读者我要写书评

暂无评论

Erlotinib Analogue-substituted Zinc（Ⅱ） Phthalocyanines for Small Molecular Target-based Photodynamic Cancer Therapy

引用

Chinese Journal of Chemistry 2016年第10期34卷 983-988页

作者： Juanjuan Chen Huannian Ye Mingjun Zhang Jinyu Li Jianyong Liu Jinping Xue state key laboratory of photocatalysis on energy and environment & fujian engineering research center of functional materials College of Chemistry Fuzhou University Fuzhou Fujian 350002 China

＂Smart＂ targeted photosensitizer conjugated with small molecule target-based anticancer drug which has a sim- ple chemical structure and high stability, is a new promising targeted therapeutic strategy. We herein extended this strategy and reported a novel series of zinc（II） phthalocyanine-erlotinib analogue conjugates with different periph- eral substituted positions and lengths of the linker. Having erlotinib analogue as the targeting moiety, all conjugates exhibited high specificity and potent affinity to HepG2 cancer cells and kept high photodynamic activity （ICs0 = 3.7 -- 16.7 nmol/L）. Structure-activity relationships of these conjugates were assessed by investigating their photophys- ical/photochemical properties, targeting intracellular uptake and in vitro phototoxicity. The results suggested that a-substituted conjugates showed slightly higher photodynamic activity than ,8-substituted ones. In conclusion, we have developed a series of promising anticancer agents with high tumor selectivity and anticancer activity for targeted photodynamic therapy.

关键词： antitumor agents targeted photodynamic therapy small molecular target-based drug erlotinib,phthalocyanines

来源：

维普期刊数据库评论

在线全文

维普期刊数据库

学校读者我要写书评

暂无评论

Selectively converting CO_(2) to HCOOH on Cu-alloys integrated in hematite-driven artificial photosynthetic cells

引用

Journal of energy Chemistry 2023年第4期79卷 601-610页

作者： Jiwu Zhao Liang Huang Lan Xue Zhenjie Niu Zizhong Zhang Zhengxin Ding Rusheng Yuan Xu Lu Jinlin Long state key laboratory of photocatalysis on energy and environment College of ChemistryFuzhou UniversityFuzhou 350116FujianChina Clean Combustion research center(CCRC) Division of Physical Sciences and EngineeringKing Abdullah University of Science and Technology(KAUST)Thuwal 23955-6900Saudi Arabia

The integration of electrochemical CO_(2)reduction(CO_(2)RR) and photoelectrochemical water oxidation offers a sustainable access to valuable chemicals and fuels. Here, we develop a rapidly annealed hematite photoanode with a photocurrent density of 2.83 mA cm^(-2)at 1.7 VRHEto drive the full-reaction. We also present Cu-alloys electrocatalysis extended from CuInSnS4, which are superior in both activity and selectivity for CO_(2)RR. Specifically, the screened CuInSn achieves a CO_(2)to HCOOH Faradaic efficiency of 93% at a cell voltage of-2.0 V by assembling into artificial photosynthesis cell. The stability test of IT exhibits less than 3% degradation over 24 h. Furthermore, in-situ Raman spectroscopy reveals that both CO_(3)^(-2)and CO_(2)are involved in CO_(2)RR as reactants. The preferential affinity of C for H in the ^(*)HCO_(2)intermediate enables an improved HCOOH-selectivity, highlighting the role of multifunctional Cu in reducing the cell voltage and enhancing the photocurrent density.

关键词： CO_(2)reduction Rapid annealing Fe_(2)O_(3)photoanode CuInSnS_(4) In-situ spectroscopy

来源：

维普期刊数据库

同方期刊数据库评论

在线全文

学校读者我要写书评

暂无评论

Modulation of lattice oxygen boosts the electrochemical activity and stability of Co-free Li-rich cathodes

引用

Journal of energy Chemistry 2022年第12期75卷 117-126,I0004页

作者： Gui-Jing Xu Wang Ke Fu-Da Yu Jie Feng Yun-Shan Jiang Lan-Fang Que Lei Zhao Zhen-Bo Wang MIIT key laboratory of Critical materials Technology for New energy Conversion and Storage School of Chemistry and Chemical EngineeringState Key Lab of Urban Water Resource and EnvironmentHarbin Institute of TechnologyHarbin 150001HeilongjiangChina engineering research center of environment-Friendly functional materials Ministry of EducationInstitute of Materials Physical ChemistryHuaqiao UniversityXiamen 361021FujianChina College of materials Science and engineering Shenzhen UniversityShenzhen 518071GuangdongChina

Co-free Li-rich layered oxide cathodes have drawn much attention owing to their low cost and high energy density.Nevertheless,anion oxidation of oxygen leads to oxygen peroxidation during the first charging process,which leads to co-migration of transition metal ions and oxygen vacancies,causing structural instability.In this work,we propose a pre-activation strategy driven by chemical impregnation to modulate the chemical state of surface lattice oxygen,thus regulating the structural and electrochemical properties of the cathodes.In-situ X-ray diffraction confirms that materials based on activated oxygen configuration have higher structural stability.More importantly,this novel efficient strategy endows the cathodes having a lower surface charge transfer barrier and higher Li+transfer kinetics characteristic and ameliorates its inherent issues.The optimized cathode exhibits excellent electrochemical performance:after 300 cycles,high capacity(from 238 m Ah g^(-1)to 193 m Ah g^(-1)at 1 C)and low voltage attenuation(168 mV)are obtained.Overall,this modulated surface lattice oxygen strategy improves the electrochemical activity and structural stability,providing an innovative idea to obtain high-capacity Co-free Li-rich cathodes for next-generation Li-ion batteries.

关键词： Pre-activation Modulation of lattice oxygen In-situ X-ray diffraction Structure stability Co-free Li-rich cathodes

来源：

维普期刊数据库

同方期刊数据库评论

在线全文

学校读者我要写书评

暂无评论

Facet effect on the reconstructed Cu-catalyzed electrochemical hydrogenation of 5-hydroxymethylfurfural(HMF) towards 2,5-bis(hydroxymethy)furan (BHMF)

引用

Journal of energy Chemistry 2023年第9期84卷 101-111页

作者： Mengxia Li Tianxi Zheng Dongfei Lu Shiwei Dai Xin Chen Xinchen Pan Dibo Dong Rengui Weng Gang Xu Fanan Wang fujian Provincial key laboratory of Advanced materials Oriented Chemical engineering College of Chemistry and Material ScienceFujian Normal UniversityFuzhou 350007FujianChina fujian Provincial key laboratory of Polymer materials College of Chemistry and Materials ScienceFujian Normal UniversityFuzhou 350007FujianChina fujian Eco-materials engineering research center School of Ecological Environment and Urban ConstructionFujian University of TechnologyFuzhou 350118FujianChina Institute of Smart Marine and engineering Fujian University of TechnologyFuzhou 350118FujianChina

The electrochemical hydrogenation of HMF to BHMF is an elegant alternative to the conventio nal thermocatalytic route for the production of high-value-added chemicals from biomass resources.In virtue of the wide potential window with promising Faradic efficiency(FE) towards BHMF,Cu-based electrode has been in the center of investigation.However,its structure-activity relationship remains ambiguous and its intrinsic catalytic activity is still unsatisfactory.In this work,we develop a two-step oxidation-reduction strategy to reconstruct the surface atom arrangement of the Cu foam(CF).By combination of multiple quasi-situ/in-situ techniques and density functional theory(DFT) calculation,the critical factor that governs the reaction is demonstrated to be facet effect of the metallic Cu crystal:Cu(110) facet accounts for the most favorable surface with enhanced chemisorption with reactants and selective production of BHMF,while Cu(100) facet might trigger the accumulation of the by-product 5,5'-bis(hydroxy methy)hydrofurion(BHH).With the optimized composition of the facets on the reconstructed Cu(OH)_(2)-ER/CF,the performance could be noticeably enhanced with a BHMF FE of 92.3% and HMF conversion of 98.5% at a potential of -0.15 V versus reversible hydrogen electrode(vs.RHE) in 0.1 M KOH solution.This work sheds light on the incomplete mechanistic puzzle for Cu-catalyzed electrochemical hydrogenation of HMF to BHMF,and provides a theoretical foundation for further precise design of highly efficient catalytic electrodes.

关键词： Electrochemical hydrogenation Biomass conversion 5-hydroxymethylfurfural Cu electrode Facet effect

来源：

维普期刊数据库

同方期刊数据库评论

在线全文

学校读者我要写书评

暂无评论

Plant-leaf-inspired MXene-silk composite for intelligent solar steam generation combined with mechanical actuation

引用

Nano research 2023年第5期16卷 7792-7800页

作者： Yongqiang Qian Zhiling Luo Yi Wang Wei Zhang Luzhuo Chen fujian Provincial key laboratory of Quantum Manipulation and New energy materials College of Physics and EnergyFujian Normal UniversityFuzhou 350117China fujian Provincial Collaborative Innovation center for Advanced High-Field Superconducting materials and engineering Fuzhou 350117China fujian Provincial engineering Technology research center of Solar energy Conversion and energy Storage Fuzhou 350117China

Solar steam generators based on photothermal materials are important in producing fresh water.However,conventional solar steam generators are difficult to self-adapt to the complex external environment as organisms.Herein,inspired by the plant leaf,we propose a photothermal composite based on MXene and silk to add more functionality.On one hand,the composite achieves an evaporation rate of 1.51 kg·m^(−2)·h^(−1)and a conversion efficiency of 86.9%under a solar intensity of 1 kW·m^(−2),mimicking the water transpiration of plant leaf.On the other hand,the MXene-silk-based actuator shows a maximum bending curvature of 0.91 cm^(−1)under a solar intensity of 5 kW·m^(−2).Furthermore,an intelligent solar system is constructed utilizing the synergy of solar steam generator and actuator,which advances the research from the material level to the system level.Mimicking the behavior of plant leaf,the system can automatically open during the day to generate steam and fresh water.And at night or in bad weather,it will automatically close to prevent external pollution such as dust,achieving intelligent anti-fouling.This research will have good application prospects in less developed areas.Meanwhile,it also provides a certain reference value for exploring multi-functional photothermal devices in the future.

关键词： MXene silk solar steam generator photothermal actuator multi-functional

来源：

维普期刊数据库评论

在线全文

维普期刊数据库

学校读者我要写书评

暂无评论

Peripheral Coordination-Dependent Descriptor for Selective Interactions between Near-Frontier Molecular Orbitals and Single-Atom Catalysts

Precision Chemistry

引用

Precision Chemistry 2023年第7期1卷 429-436页

作者： Bingqing Ge Fenfei Wei Qiang Wan Hongwei Zhang Pei Yuan Sen Lin state key laboratory of photocatalysis on energy and environment College of Chemistry and National Engineering Research Center of Chemical Fertilizer CatalystCollege of Chemical EngineeringFuzhou UniversityFuzhou 350002China state key laboratory of photocatalysis on energy and environment College of ChemistryFuzhou UniversityFuzhou 350002China National engineering research center of Chemical Fertilizer Catalyst College of Chemical EngineeringFuzhou UniversityFuzhou 350002China

Selective adsorption of α,β-unsaturated aldehydes(α,β-UALs)is a prerequisite for the hydrogenation of α,β-UALs to high-value unsaturated alcohols,but a quantitative description of the interactions between the C=C/C=O bond of α,β-UALs and the catalysts is still lacking.Herein,based on comprehensive density functional theory calculations,we developed a descriptor that combines the near-frontier molecular orbitals of the C=C/C=O bonds of α,β-UALs with the fundamental physical properties of single-atom catalysts(SACs)and considers the inner/outer coordination environment.All of the parameters used in this descriptor are easily accessible and interpretable,enabling an efficient assessment of the selectivity of SACs for the C=C/C=O bonds ofα,β-UALs.

关键词： selectivity adsorption coordination environment DFT descriptor

来源：

维普期刊数据库评论

在线全文

维普期刊数据库

学校读者我要写书评

暂无评论

How water molecules occupying the active site of a single-atom catalyst affect the electrochemical reduction of carbon dioxide

引用

Nano research 2023年第7期16卷 9091-9098页

作者： Jia Zhao Di Liu Fenfei Wei Weng Fai Ip Hui Pan Sen Lin state key laboratory of photocatalysis on energy and environment College of ChemistryFuzhou UniversityFuzhou 350002China Institute of Applied Physics and materials engineering University of MacaoTaipa 999078MacaoChina Department of Physics and Chemistry Faculty of Science and TechnologyUniversity of MacaoTaipa 999078MacaoChina

In single-atom catalysts(SACs),the single atoms are often exposed as protrusions above the substrate.The solvent molecules in the electrocatalytic environment can interact or even bind to these coordination-unsaturated single atoms and thus influence the reaction process,but this has not been studied in depth.In this work,we systematically investigate the thermodynamics of CO_(2)reduction reaction(CO_(2)RR)to CO over MoS_(2)-supported single metal atom catalysts(TM@MoS_(2),TM=transition metal)under vacuum and explicit solvent environments using density functional theory.In addition,the ab initio molecular dynamics results show that explicit H_(2)O molecules can coordinate to the TM site and undergo competitive adsorption with the CO_(2)RR intermediates,which significantly affects the energy and conformation of the CO_(2)RR pathway.Electronic structure analysis reveals that the occupying H_(2)O molecules change the electronic state of single atom and further influence the adsorption strength of different CO_(2)RR intermediates.Our work shows that water molecules can not only act as ligands to influence the electronic state of TM,but also affect the energy and conformation of CO_(2)RR intermediates,which highlights the important role of occupying H_(2)O molecules at the single-atom sites in CO_(2)RR and provides useful insights for the design of SACs for efficient CO_(2)RR.

关键词： electrocatalytic CO_(2)reduction solvent effect single-atom catalysis density functional theory ab initio molecular dynamics

来源：

维普期刊数据库评论

在线全文

维普期刊数据库

学校读者我要写书评

暂无评论

欢迎您,

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

在线全文

在线全文

在线全文

在线全文

在线全文

在线全文

在线全文

在线全文

在线全文

在线全文

请选择保存的检索档案：

请选择收藏分类：

通借通还

欢迎您,

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

在线全文

在线全文

在线全文

在线全文

在线全文

在线全文

在线全文

在线全文

在线全文

在线全文

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：