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In situ meso-tetra(4-carboxyphenyl)porphyrin ligand substitution in Hf-MOF for enhanced catalytic activity and stability in photoredox reactions

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Rare Metals 2024年第6期43卷 2682-2694页

作者： Jie hu hong-Xin Lao Xiu-Wu Xu Wei-Kang Wang Le-Le Wang Qin-Qin Liu School of Materials Science and Engineering Jiangsu UniversityZhenjiang 212013China College of Chemistry and Materials Engineering Research Center of Carbon NeutralityAnhui Normal UniversityWuhu 241002China Fujian Provincial Key Laboratory of Ecology-Toxicological Effects and Control for Emerging Contaminants Putian UniversityPutian 351100China

Though there are numerous intrinsic merits of metal-organic frameworks(MOFs),low charge separation efficiency has imposed heavy restrictions on their photocatalytic ***,in situ porphyrin ligand substitution,as a strategy for improving the charge separation efficiency and increasing the amounts of active sites,has been designed and realized in a Hf-biphenyl dicarboxylic acid(BPDC)***,a size and geometry matched meso-tetra(4-carboxyphenyl)porphyrin(TCPP)ligand was selected and doped into Hf-BPDC MOF by forming coordinating bonds with Hf centers,forming dualligand Hf-BPDC-TCPP *** resultant Hf-BPDC-TCPP MOF showed significantly improved activity and chemical stability in the photocatalytic H_(2)generation(261μmol·g^(-1)·h^(-1))and tetracycline(TC)degradation reactions(95.8%),which was 48 and 1.47 folds higher than that of the Hf-BPDC *** and electrochemical studies revealed that the introduction of porphyrin ligand could generate a stronger internal electric field for boosting the charge separation and transfer,increase the specific surface area for providing more active sites,and narrow the band gap to enhance the visible light *** in situ ligand substitution method provides a promising approach to build a tunable platform for constructing high-performance MOF photocatalysts.

关键词： Ligand substitution Metal organic frameworks Meso-tetra(4-carboxyphenyl)porphyrin Hydrogen evolution reaction Tetracycline degradation

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Spin effect on redox acceleration and regioselectivity in Fe-catalyzed alkyne hydrosilylation

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National Science Review 2024年第2期11卷 155-167页

作者： Peng He Meng-Yang hu Jin-hong Li Tian-Zhang Qiao Yi-Lin Lu Shou-Fei Zhu Frontiers Science Center for New Organic Matter State Key Laboratory and Institute of Elemento-Organic Chemistry Nankai University

Iron catalysts are ideal transition metal catalysts because of the Earths abundant, cheap, biocompatible features of iron salts. Iron catalysts often have unique open-shell structures that easily undergo spin crossover in chemical transformations, a feature rarely found in noble metal catalysts. Unfortunately, little is known currently about how the open-shell structure and spin crossover affect the reactivity and selectivity of iron catalysts, which makes the development of iron catalysts a low efficient trial-and-error program. In this paper, a combination of experiments and theoretical calculations revealed that the iron-catalyzed hydrosilylation of alkynes is typical spin-crossover catalysis. Deep insight into the electronic structures of a set of well-defined open-shell active formal Fe(0) catalysts revealed that the spin-delocalization between the iron center and the 1,10-phenanthroline ligand effectively regulates the iron center's spin and oxidation state to meet the opposite electrostatic requirements of oxidative addition and reductive elimination, respectively,and the spin crossover is essential for this electron transfer process. The triplet transition state was essential for achieving high regioselectivity through tuning the nonbonding interactions. These findings provide an important reference for understanding the effect of catalyst spin state on reaction. It is inspiring for the development of iron catalysts and other Earth-abundant metal catalysts, especially from the point of view of ligand development.

关键词： spin effect spin-delocalization spin crossover iron-catalysis alkyne hydrosilylation

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Supporting IrO_(x) nanosheets on hollow TiO_(2) for highly efficient acidic water splitting

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Nano Research 2024年第8期17卷 6903-6909页

作者： Ge Yu Ruilong Li Yanmin hu Xingen Lin Ze Lin Dongyang Wu Gongming Wang Xun hong Center of Advanced Nanocatalysis(CAN) Department of Applied ChemistryUniversity of Science and Technology of ChinaHefei 230026China

The efficiency of proton exchange membrane water electrolysis(PEM-WE)for hydrogen production is heavily dependent on the noble metal iridium-based ***,the scarcity of iridium limits the large-scale application of *** address this issue,it is promising to select an appropriate support because it not only enhances the utilization efficiency of noble metals but also improves mass transport under high ***,we supported amorphous IrO_(x) nanosheets onto the hollow TiO_(2) sphere(denoted as IrO_(x)),which demonstrated excellent performance in acidic electrolytic water ***,the annealed IrO_(x)catalyst at 150℃in air exhibited a mass activity of 1347.5 A·gIr^(−1),which is much higher than that of commercial IrO_(2) of 12.33 A·gIr^(−1) at the overpotential of 300 mV for oxygen evolution reaction(OER).Meanwhile,the annealed IrO_(x) exhibited good stability for 600 h operating at 10 mA·cm^(−2).Moreover,when using IrO_(x) and annealed IrO_(x) catalysts for water splitting,a cell voltage as low as 1.485 V can be achieved at 10 mA·cm^(−2).The cell can continuously operate for 200 h with negligible degradation of performance.

关键词： oxygen evolution reaction hydrogen evolution reaction amorphous IrO_(x) hollow TiO_(2) proton exchange membrane water electrolysis

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Application of a concrete thermal pile in cooling the warming permafrost under climate change

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Advances in Climate Change Research 2024年第1期15卷 170-183页

作者： Yun-hu SHANG Fu-Jun NIU Guo-Yu LI Jian-hong FANG Ze-Yong GAO State Key Laboratory of Frozen Soil Engineering Northwest Institute of Eco-Environment and ResourcesChinese Academy of SciencesLanzhou 730000China Da Xing'anling Observation and Research Station of Frozen-Ground Engineering and Environment Northwest Institute of Eco-Environment and ResourcesChinese Academy of SciencesJagdaqi 165000China Qinghai Research Institute of Transportation Xining 810008China

Permafrost degradation caused by climate warming is posing a serious threat to the stability of cast-in-place pile foundations in warm permafrost *** cold energy can be effectively utilized by two-phase closed thermosyphons(TPCTs)to cool the ***,we installed TPCTs in a cast-in-place pile foundation to create a unique structure called a thermal pile,which effectively utilizes the TPCTs to regulate ground *** we conducted a case study and numerical simulation to exhibit the cooling performance,and optimize the structure of the thermal *** purpose of this study is to promote the application of thermal piles in unstable permafrost *** on the findings,the thermal pile operated for approximately 53%of the entire year and effectively reduced the deep ground temperature at a rate of at least-0.1℃per ***,it successfully raised the permafrost table that is 0.35 m shallower than the natural ground *** characteristics prove highly beneficial in mitigating the adverse effects of permafrost degradation and enhancing infrastructure *** the length of the condenser section and the diameter of the TPCT in a suitable manner can effectively enhance the cooling capability of the thermal pile and ensure the long-term mechanical stability of the pile foundation even under climate warming.

关键词： Heat transfer Cold energy Warm permafrost Two-phase closed thermosyphons Cast-in-place pile foundation

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Experimental Study on Vortex-Induced Vibration of Rough Risers with Coupling Interference Effect Under Side-by-Side Arrangement

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China Ocean Engineering 2024年第1期38卷 18-28页

作者： hu Ze-bo LIU Zhen LI Peng GUO Hai-yan WANG Shu-bing REN Xiao-hui HOU Hao WANG ye-shuo College of Civil Engineering and Architecture Shandong University of Science and TechnologyQingdao 266590China Qingdao Key Laboratory of Marine Civil Engineering Materials and Structures Qingdao 266590China College of Engineering Ocean University of ChinaQingdao 266100China CHEC Dredging Co. LtdShanghai 200136China

A vortex-induced vibration(VIV)experiment of rough risers with coupling interference effect under a side-by-side arrangement was carried out in a wave-current combined *** roughness of the riser was characterized by arranging different specifications of surface attachments on the surface of the *** risers with three different roughnesses were arranged side by side with smooth risers to explore the VIV response of the riser under the combined action of roughness and interference effect,and to reveal the coupling mechanism between roughness and interference *** experimental results show that,compared with that of a smooth riser,the VIV of a rough riser under the coupling interference effect has a wider"lock-in"region,and the displacement decreases more significantly at a high reduced velocity,which is more likely to excite higher-order modes and frequency *** addition,the displacement response and frequency response of the smooth riser are not significantly affected by wake interference from the rough riser,which is caused by the decrease of the wake region due to the delay of the boundary layer separation point of the rough riser.

关键词： marine riser vortex-induced vibration side-by-side arrangement roughness interference effect

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Two new high-temperature molecular ferroelectrics[1,5-3.2.2-Hdabcn]X(X=ClO_(4)^(-),ReO_(4)^(-))

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Chinese Chemical Letters 2024年第6期35卷 234-238页

作者： Keke Han Wenjun Rao Xiuli You Haina Zhang Xing ye Zhenhong Wei hu Cai School of Chemistry and Chemical Engineering Nanchang UniversityNanchang 330031China Jiangxi Key laboratory of Organic Chemistry Jiangxi Science and Technology Normal UniversityNanchang 330013China

Molecular ferroelectrics have attracted much attention because of their excellent piezoelectricity,mechanical workability,and second harmonic ***,we successfully prepared two molecular ferroelectrics[1,5-3.2.2-Hdabcn]X(X=ClO_(4)^(-),1;ReO_(4)^(-),2)by reactions of a quasi-spherical amine 1,5-diazabicycle[3.2.2]nonane(1.5-3.2.2-dabcn)with HX aqueous *** 1 and 2 undergo hightemperature phase transitions at 381 K(1)and 396 K(2).Before and after the phase transition,they crystallize in the polar point group mm2,and the centrosymmetric point groups mmm and 4/mmm,*** to Aizu rules,these two compounds experience mmm Fmm2 and 4/mmm Fmm2 type ferroelectric phase transitions,*** ferroelectricity of both compounds is well expressed in their polycrystalline film at room temperature with low coercive voltages of 13 V for 1 and 25 V for *** piezoelectric force microscopy(PFM),the 180°anti-parallel ferroelectric domains and the reversible polarization switching can be clearly observed in 1 and *** high-temperature molecular ferroelectric material has great application potential in flexible materials,biomechanics,intelligent wearables and other fields.

关键词： Ferroelectric domains Quasi-spherical amine Phase transition Polarization

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Metal size effects over metal/zeolite bifunctional catalysts in the selective hydroalkylation of benzene

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Frontiers of Chemical Science and Engineering 2024年第4期18卷 107-114页

作者： Junjie Li Chuang Liu Zhenlong Jia Yingchun ye Dawei Lan Wei Meng Jianqiang Wang Zhendong Wang Yongfeng hu Weimin Yang State Key Laboratory of Green Chemical Engineering and Industrial Catalysis Sinopec Shanghai Research Institute of Petrochemical Technology Co.Ltd.Shanghai 201208China School of Chemical Engineering East China University of Science and TechnologyShanghai 200237China

Bifunctional metal/zeolite materials are some of the most suitable catalysts for the direct hydroalkylation of benzene to *** overall catalytic performance of this reaction is strongly influenced by the hydrogenation,which is dependent on the metal ***,systematically investigating the metal size effects in the hydroalkylation of benzene is *** this work,we successfully synthesized Ru and Pd nanoparticles on Sinopec Composition Materials No.1 zeolite with various metal *** demonstrated the size-dependent catalytic activity of zeolite-supported Ru and Pd catalysts in the hydroalkylation of benzene,which can be attributed to the size-induced hydrogen spillover capability *** work presents new insights into the hydroalkylation reaction and may open up a new avenue for the smart design of advanced metal/zeolite bi-functional catalysts.

关键词： size effects bifunctional catalysts metal/zeolite hydroalkylation

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The structure of TRAF7 coiled-coil trimer provides insight into its function in zebrafish embryonic development

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Journal of Molecular Cell Biology 2024年第1期16卷 43-53页

作者： Xiaozhen Song Ruixing hu Yi Chen Man Xiao hong Zhang Shengnan Wu Qing Lu Molecular Diagnostic Laboratory Shanghai Children’s HospitalSchool of MedicineShanghai Jiao Tong UniversityShanghai 200040China Bio-X Institutes Key Laboratory for the Genetics of Developmental and Neuropsychiatric Disorders(Ministry of Education)Shanghai Jiao Tong UniversityShanghai 200030China Laboratory of Development and Diseases and State Key Laboratory for Medical Genomics Shanghai Institute of HematologyRuĳin HospitalShanghai JiaoTong University School of MedicineShanghai 200025China

TRAF7 serves as a crucial intracellular adaptor and E3 ubiquitin ligase involved in signal transduction pathways,contributing to immune responses,tumor progression,and embryonic *** mutations within the coiled-coil(CC)domain and WD40 repeat domain of TRAF7 could cause brain tumors,while germline pathogenic mutations contribute to severe developmental ***,the precise molecular mechanism underlying TRAF7 involvement in embryonic development remains *** this study,we employed zebrafish as an in vivo model ***7 knock down caused defects in zebrafish embryonic *** determined the crystal structure of TRAF7 CC domain at 3.3Åresolution and found that the CC region trimerization was essential for TRAF7 functionality during zebrafish embryonic ***,disease-causing mutations in TRAF7 CC region could impair the trimer formation,consequently impacting early embryonic development of ***,our study sheds light on the molecular mechanism of TRAF7 CC trimer formation and its pivotal role in embryonic development.

关键词： TRAF7 coiled-coil domain crystal structure trimerization embryonic development

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Pd@Ir-LOD multienzyme utilizing endogenous lactate consumption cooperates with photothermal for tumor therapy

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Nano Research 2024年第1期17卷 270-281页

作者： Zichen ye Yun Li Jingchao Li Xinyan hu Jinyang Zheng Gongxin Zhang Sijin Xiang Tianbao Zhu Zhide Guo Xiaolan Chen State Key Laboratory for Physical Chemistry of Solid Surfaces Collaborative Innovation Center of Chemistry for Energy Materials and Engineering Research Center for Nano-Preparation Technology of Fujian ProvinceCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China State Key Laboratory of Molecular Vaccinology and Molecular Diagnostics&Center for Molecular Imaging and Translational Medicine School of Public Health Xiamen UniversityXiamen 361102China The High Educational Key Laboratory for Biomedical Engineering&Key Laboratory of Fire Retardant Materials of Fujian Province Department of BiomaterialsCollege of MaterialsXiamen UniversityXiamen 361102China

Lactic acid(LA)plays a major role in the occurrence,development,and spread of *** by its high accumulation in tumor site,a novel lactate oxidase(LOD)conjugated two-dimensional Pd@Ir nanoplatform(Pd@Ir-LOD,PIL)was fabricated to combine cascade reaction with photothermal for tumor *** detail,the overexpressed LA in tumor microenvironment(TME)was a key factor to activate the PIL-based cascade reaction:(1)Plenty of H_(2)O_(2)could be generated from LA by the catalysis of LOD with O_(2);(2)potent·OH was produced from H_(2)O_(2)due to the peroxidase(POD)-like activity of PIL;(3)meantime,PIL’s catalase(CAT)-like activity could decompose part H_(2)O_(2)into O_(2)to achieve the purpose of LA cyclic ***,the reduced glutathione(GSH)scavenging capability of PIL might protect the produced reactive oxygen species(ROS)from being cleared to further improve the cascade therapeutic *** importantly,PIL had excellent photothermal conversion efficiency(37.35%)and manifested a surprising temperature rising effect in *** together,the decreasing LA concentration,accumulation of high-toxic ROS,the depletion of GSH together with the higher intra-tumoral temperature potently enhanced in vivo antitumor ***,a promising therapeutic tactic based on PIL integrating endogenous LA consumption,chemodynamic therapy(CDT),and photothermal therapy(PTT)has been put forward.

关键词： lactate oxidase chemodynamic therapy photothermal therapy cascade reaction tumor microenvironment

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Approaching the theoretical capacity of TiO_(2) anode in a photorechargeable lithium-ion battery

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Nano Research 2024年第4期17卷 2655-2662页

作者： Wen Yan Jie Wang Qing hu Jingjing Fu Mohamed K.Albolkany Tian Zhang Xiao Lu Fei ye Bo Liu School of Chemistry and Materials Science University of Science and Technology of ChinaHefei 230026China

New generation of lithium-ion batteries(LIBs)integrating solar energy conversion and storage is emerging,as they could solve the fluctuation problem in the utilization of solar ***-rechargeable lithium-ion batteries(PR-LIBs)are ideal devices for such target,in which solar energy is converted into electricity and stored in *** order to achieve the high performance of PR-LIB,it is crucial to develop dual-function electrode materials that can synergistically capture solar energy and store ***,we present photo-rechargeable lithium-ion batteries using defective black TiO_(2) as photoanode prepared by lithium *** photoanode exhibits excellent photo response in full solar spectrum with a capacity enhancement of 46.4%under illumination,corresponding to the energy conversion efficiency of 4.4%at the current density of 1 A·g^(-1).When illumination is applied at 20 mA·g^(-1),the battery capacity increases from~230 in dark to~349 mAh·g^(-1) at the first cycle,and then stabilizes at 310 mAh·g^(-1),approaching the theoretical value of 335 mAh·g^(-1) of TiO_(2) electrode *** finding provides thoughts for breaking the capacity limitations in TiO_(2) and paves the way for powering LIBs by solar illumination.

关键词： photo-rechargeable lithium-ion batteries photoanode defective TiO_(2)(D-TiO_(2))

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