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Covalence bridge atomically precise metal nanocluster and metalorganic frameworks for enhanced photostability and photocatalysis

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Nano Research 2023年第1期16卷 1527-1532页

作者： Aimin Yao Yuanxin Du Meng Han Yan Wang Jiashen Hu Qingtao Zhu Hongting Sheng Manzhou Zhu Department of materials Science and engineering Centre for Atomic Engineering of Advanced MaterialsKey Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of EducationKey Laboratory of Functional Inorganic Material Chemistry of Anhui ProvinceAnhui UniversityHefei 230601China

Metal nanoclusters(NCs)with precise structure and ultrasmall size have attracted great interests in catalysis.However,the poor stability has limited its large-scale use.Herein,we proposed the“covalence bridge”strategy to effectively connect atomically precise metal NCs and metal-organic frameworks.Benefiting from the covalent linkage,the synthesized UiO-66-NH2-Au25(LCys)18 showed outstanding stability after 16 h photocatalysis.Moreover,the covalence bridge created a strong metal-support interaction between the two components and provided an effective charge transport channel and thereby enhanced photocatalytic activity.UiO-66-NH2-Au25(L-Cys)18 displayed an exceptional photocatalytic H2 production rate,which is 21 and 90 times higher than that of UiO-66-NH2/Au25(PET)18(made by physically combination)and bare UiO-66-NH2,respectively.Thermodynamic and kinetic studies demonstrated that UiO-66-NH2-Au25(L-Cys)18 exhibited higher charge transfer efficiency,lower overpotential of water reduction and activation energy barrier compared with its counterparts.

关键词： atomically precise nanoclusters metal-organic frameworks covalent binding photostability photocatalytic hydrogen production

Two dimensional MoS_(2) finding its way towards constructing high-performance alkaline recovery membranes

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中国化学工程学报:英文版 2023年第8期60卷 155-164页

作者： Xinxin Li Hongwei Shao Shichao Zhang Yong Li Jingjing Gu Qiang Huang Jin Ran anhui key laboratory of Advanced Catalytic materials and Reaction engineering School of Chemistry and Chemical EngineeringHefei University of TechnologyAnhui 230009China

The available alkaline recovery membranes are currently dominated by polymeric materials,but they suffer from a permeation-selectivity trade-off and inferior chemical resistance.Robust two dimensional(2D) lamellar membranes with sub-nanometer wide channels are promising candidates for discerning OH^(-)and other anions.Here,we report the development of alkaline recycling membranes through stacking MoS_(2) nanosheets.Benefiting from the ordered and narrow 2D channels,MoS_(2) membranes show excellent alkaline recovery performances.The OH^(-)dialysis coefficient (U_(OH)-) and separation factor (S)towards simulated OH^(-) and WO_(4)^(2-) across the 500 nm thick MoS_(2) laminates reach 6.9×10^(-3)m·h^(-1)and 34.3 respectively.Furthermore,the chemical environments of MoS_(2) laminates were modulated by intercalating ionic poly(sodium 4-styrene sulfonate)(PSS@MoS_(2)).The U_(OH)-and S values of PSS@MoS_(2) membrane further improve to 11.7×10^(-3)m·h^(-1)and 49.8 respectively.Besides,both MoS_(2) and PSS@MoS_(2) membranes exhibit promising stability.

关键词： Alkaline recovery Diffusion dialysis Two dimensional membranes MoS_(2) Poly(sodium 4-styrene sulfonate)

Theoretical investigation on NO reduction electro-catalyzed by transition-metal-anchored SnOSe nanotubes

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Nano Research 2023年第7期16卷 8533-8541页

作者： Renqiang Zhao Zengying Ma Yanghong Yu Xueqian Xia Bowen Song Tao Zhou Yucheng Huang College of Chemistry and Material Science Key Laboratory of Electrochemical Clean Energy of Anhui Higher Education InstitutesKey Laboratory of Functional Molecular SolidsMinistry of EducationAnhui Key Laboratory of Molecule-Based MaterialsAnhui Provincial Engineering Laboratory of New-Energy Vehicle Battery Energy-Storage MaterialsAnhui Carbon Neutrality Engineering CenterAnhui Normal UniversityWuhu 241000China

Electrochemical NO reduction reaction(NORR)to NH3 emerges as a fascinating approach to achieve both the migration of NO pollutant and the green synthesis of NH3.In this contribution,within the framework of computational hydrogen model and constant-potential implicit solvent model,the NORR electrocatalyzed by a novel transition-metal-anchored SnOSe armchair nanotube(TM@SnOSe_ANT)was investigated using density functional theory calculations.Through the checking in terms of stability,activity,and selectivity,Sc-and Y@SnOSe_ANTs were screened out from the twenty-five candidates.Considering the effects of pH,solvent environment,as well as applied potential,only Sc@SnOSe_ANT is found to be most promising.The predicted surface area normalized capacitance is 11.4μF/cm^(2),and the highest NORR performance can be achieved at the U_(RHE) of-0.58 V in the acid environment.The high activity originates from the mediate adsorption strength of OH.These findings add a new perspective that the nanotube can be served as a highly promising electrocatalyst towards NORR.

关键词： nanotube SnOSe electrochemical NO reduction ammonia synthesis NO removal constant-potential implicit solvent model density functional theory calculation

Rationally construction of atomic-precise interfacial charge transfer channel and strong build-in electric field in nanocluster-based Zscheme heterojunctions with enhanced photocatalytic hydrogen production

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Nano Research 2024年第6期17卷 5002-5010页

作者： Qingtao Zhu Honglei Shen Chao Han Liu Huang Yanting Zhou Yuanxin Du Xi Kang Manzhou Zhu Department of materials Science and engineering Centre for Atomic Engineering of Advanced MaterialsKey Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of EducationKey Laboratory of Functional Inorganic Material Chemistry of Anhui ProvinceAnhui UniversityHefei 230601China

The lack of effective charge transfer driving force and channel limits the electron directional migration in nanoclusters(NC)-based heterostructures,resulting in poor photocatalytic performance.Herein,a Z-scheme NC-based heterojunction(Pt1Ag28-BTT/CoP,BTT=1,3,5-benzenetrithiol)with strong internal electric field is constructed via interfacial Co-S bond,which exhibits an absolutely superiority in photocatalytic performance with 24.89 mmol·h^(−1)·g−1 H_(2)production rate,25.77%apparent quantum yield at 420 nm,and~100%activity retention in stability,compared with Pt1Ag28-BDT/CoP(BDT=1,3-benzenedithiol),Ag29-BDT/CoP,and CoP.The enhanced catalytic performance is contributed by the dual modulation strategy of inner core and outer shell of NC,wherein,the center Pt single atom doping regulates the band structure of NC to match well with CoP,builds internal electric field,and then drives photogenerated electrons steering;the accurate surface S modification promotes the formation of Co-S atomic-precise interface channel for further high-efficient Z-scheme charge directional migration.This work opens a new avenue for designing NC-based heterojunction with matchable band structure and valid interfacial charge transfer.

关键词： atomically precise metal nanocluster Z-scheme heterojunction interfacial charge transfer build-in electric field photocatalytic hydrogen production

Fabrication of 3D hollow acorn-shell-like PtBi intermetallics via a surfactant-free pathway for efficient ethylene glycol electrooxidation

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Nano Research 2023年第5期16卷 6560-6567页

作者： Tingting Wan Xin Huang Sichen Li Qiuyu Li Xianlong Yang Zhenjie Sun Dong Xiang Kun Wang Peng Li Manzhou Zhu Department of Chemistry and Center for Atomic engineering of Advanced materials School of Materials Science and EngineeringAnhui Province Key Laboratory of Chemistry for Inorganic/Organic Hybrid Functionalized MaterialsAnhui UniversityHefei 230601China key laboratory of Structure and Functional Regulation of Hybrid materials Ministry of EducationAnhui UniversityHefei 230601China

The synthesis of atomically ordered Pt-based intermetallic electrocatalysts for the direct alcohol fuel cells generally requires the addition of surfactants or the high-temperature annealing.However,some residual surfactants on the surface of the assynthesized catalysts would prevent the exposure of catalytic active sites,the high-temperature annealing process is easy to accelerate the sintering of the metal,which both lead to the decline of electrocatalytic performance.Herein,we construct the atomically ordered bimetallic PtBi intermetallics with clean surfaces and unique three-dimensional hollow acorn-shell-like structure(3D PtBi HASL)by a simple,low-temperature,surfactant-free one-pot synthetic approach.Benefiting from the special hollow structures,the obtained 3D PtBi HASL intermetallics expose abundant accessible active sites.Moreover,the introduction of oxophilic metal Bi can enhance adsorption of OHads,thereby significantly facilitating removal of poisoned intermediates.Density functional theory(DFT)simulations further indicate that formation of the PtBi intermetallic phase with the downshift of the Pt d-band center endows 3D Pt49.4Bi50.6 HASL intermetallics with significantly attenuated COads and enhanced OHads adsorption,bringing about the boosting electrocatalytic property.The mass activity of the 3D Pt49.4Bi50.6 HASL intermetallics for ethylene glycol oxidation reaction is as high as 24.67 A·mgPt^(−1),which is 12.98 times higher than that of commercial Pt/C(1.90 A·mgPt^(−1)).This work may inspire the design of Pt-based intermetallics as high-efficiency anode electrocatalysts for fuel cell applications.

关键词： surfactant-free strategy PtBi intermetallic three-dimensional hollow structure electrocatalyst ethylene glycol oxidation reaction

Co-based MoF derived metal catalysts: from nano-level to atom-level

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钨科技(英文) 2023年第2期5卷 201-216页

作者： Yuan-Xin Du Yan-Ting Zhou Man-Zhou Zhu College of materials Science and engineering and anhui Province key laboratory of Chemistry for Inorganic/Organic Hybrid Functionalized materials Department of Chemistry and Center for Atomic Engineering of Advanced MaterialsKey Laboratory of Structure and Functional Regulation of Hybrid Materials of the Ministry of EducationAnhui UniversityHefei 230601China

Co-based metal-organic framework(MOF),a kind of porous crystal material composed of Co ions and organic linkers,is a common type of MOF.It not only has the intrinsic properties of MOF,such as structural diversity,functional adjustability,and high surface area,but more importantly,it contains Co metal species,which are considered by many reports to be active catalytic centers for many reactions.Meanwhile,metal catalysts always received wide and sustained attention.The combi-nation of the two types of catalysts can enhance the catalytic performance and achieve the"1+1>2"effect.In this review,we mainly overview the synthesis methods of Co-based MOF-derived metal catalysts from nano-to atom-level and their applications in the catalysis field in recent years and put forward our own views and prospects for this research direction.

关键词： Metal-organic framework Cobalt Catalysis Nanoparticle Nanocluster Single-atom catalyst

Structural performance of a façade precast concrete sandwich panel enabled by a bar-type basalt fiber-reinforced polymer connector

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Frontiers of Structural and civil engineering 2023年第1期17卷 122-137页

作者： Junqi HUANG Qing JIANG Xun CHONG Xianguo YE Caihua LIU School of civil and Hydraulic engineering Hefei University of TechnologyHefei 230009China anhui civil engineering Structures and materials laboratory Hefei 230009China

In this study,a novel diagonally inserted bar-type basalt fiber reinforced polymer(BFRP)connector was proposed,aiming to achieve both construction convenience and partially composite behavior in precast concrete sandwich panels(PCSPs).First,pull-out tests were conducted to evaluate the anchoring performance of the connector in concrete after exposure to different temperatures.Thereafter,direct shear tests were conducted to investigate the shear performance of the connector.After the test on the individual performance of the connector,five façade PCSP specimens with the bar-type BFRP connector were fabricated,and the out-of-plane flexural performance was tested under a uniformly distributed load.The investigating parameters included the panel length,opening condition,and boundary condition.The results obtained in this study primarily indicated that 1)the bar-type BFRP connector can achieve a reliable anchorage system in concrete;2)the bar-type BFRP connector can offer sufficient stiffness and capacity to achieve a partially composite PCSP;3)the boundary condition of the panel considerably influenced the out-of-plane flexural performance and composite action of the investigated façade PCSP.

关键词： precast concrete sandwich panel basalt fiber reinforced polymer pull-out performance shear performance out-of-plane flexural performance

超高性能混凝土钢纤维-基体界面黏结性能研究综述

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engineering 2023年第3期22卷 215-232页

作者：邓毓琳张祖华史才军吴泽媚张超慧 key laboratory for Green&Advanced civil engineering materials and Application Technology of Hunan Province College of Civil EngineeringHunan UniversityChangsha 410082China key laboratory of Advanced civil engineering materials of Ministry of Education School of Materials Science and EngineeringTongji UniversityShanghai 201804China

超高性能混凝土(UHPC)是一种相对较新的水泥混凝土复合材料,由于其优异的机械强度和耐久性,在基础设施建设中具有巨大的应用潜力。钢纤维与基体的界面黏结性能是决定UHPC其他力学性能的主要因素,包括抗拉、抗折、抗压强度和破坏模式(断... 详细信息

超高性能混凝土(UHPC)是一种相对较新的水泥混凝土复合材料,由于其优异的机械强度和耐久性,在基础设施建设中具有巨大的应用潜力。钢纤维与基体的界面黏结性能是决定UHPC其他力学性能的主要因素,包括抗拉、抗折、抗压强度和破坏模式(断裂行为)。本文通过讨论并比较多种纤维拉拔测试方法和分析模型,全面综述了UHPC的纤维-基体黏结行为的研究进展;详细确定并讨论了影响纤维-基体黏结的参数,包括纤维的几何形状和方向、表面处理、基体的组成和强度。最后,基于现有研究,对未来UHPC增强方法和测试细节提出了建议。

关键词： Ultra-high performance concrete Interfacial bond Steel fiber Pullout behavior

Influence of Associated Cations on the Transport and Adsorption of Chloride Ions in the Nano-channel of Calcium Aluminosilicate Hydrate Gel:A Molecular Dynamics Study

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Journal of Wuhan University of Technology(materials Science) 2022年第5期37卷 963-976页

作者：杨军 ZHANG Gaozhan 丁庆军 WANG Aiguo HOU Dongshuai anhui Province engineering laboratory of Advanced Building materials School of Materials and Chemical EngineeringAnhui Jianzhu UniversityHefei230601China State key laboratory of Silicate materials for Architectures School of Materials Science and EngineeringWuhan University of TechnologyWuhan430070China School of materials Science and engineering Department of Civil EngineeringQingdao University of TechnologyQingdao266033China

Molecular dynamics simulation was utilized to investigate the transport and adsorption of chloride in the nanopore of calcium aluminosilicate hydrate(C-A-S-H)with associated cation types of Ca,Mg,Na and K.The local ionic structure,atomic dynamics and bond stability were analyzed to elucidate the interaction between cations and chloride ions.The results show that interfacial chloride is absorbed through the ion pairing formation in the vicinity of C-A-S-H substrate.Interfacial cations can simultaneously interact aluminosilicate chains,water molecules and Cl^(-)ions,which restrict the motion of interfacial Cl^(-)ions.Pore solution chloride can be immobilized through the solvation effect of cations.Cations along with their hydration shell can connect to neighboring Cl^(-)ions to decrease their mobility.Owing to the varied ionic chemistry,cations show different interaction strength with neighboring water molecules and anions,which determines the chloride transport behavior in the nanopore of C-A-S-H.The chloride immobilization capacity of C-A-S-H nanopore with different associated cations is listed in following order:Mg^(2+)Ca^(2+)

关键词： calcium aluminosilicate hydrate nanometer channel confinement chloride immobilization associated cations ionic structure