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Integration of morphology and electronic structure modulation on cobalt phosphide nanosheets to boost photocatalytic hydrogen evolution from ammonia borane hydrolysis

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Green Energy & Environment 2024年第2期9卷 333-343页

作者： Chao Wan Yu Liang Liu Zhou Jindou Huang Jiapei Wang Fengqiu Chen Xiaoli Zhan Dang-guo Cheng School of Chemistry and Chemical Engineering Anhui Province Key Laboratory of Coal Clean Conversion and High Valued UtilizationAnhui University of TechnologyMa'anshan243002China College of Chemical and Biological Engineering Zhejiang UniversityZhejiang Provincial Key Laboratory of Advanced Chemical Engineering Manufacture Technology38 Zheda RoadHangzhou310027China Key Laboratory of New Energy and Rare Earth Resource Utilization of State Ethnic Affairs Commission Key Laboratory of Photosensitive Materials&Devices of Liaoning ProvinceSchool of Physics and Materials EngineeringDalian Nationalities University 18 Liaohe West RoadDalian116600China Institute of Zhejiang University-Quzhou 78 Jiuhua Boulevard NorthQuzhou324000China Jiangsu Key Laboratory of Advanced Catalytic Materials and Technology Changzhou University213164China

The controllable and safe hydrogen storage technologies are widely recognized as the main bottleneck for the accomplishment of sustainable hydrogen *** borane(AB)has regarded as a competitive candidate for chemical hydrogen ***,developing efficient yet high-performance catalysts towards hydrogen evolution from AB hydrolysis remains an enormous ***,cobalt phosphide nanosheets are synthesized by a facile salt-assisted along with low-temperature phosphidation strategy for simultaneously modulating its morphology and electronic structure,and function as hydrogen evolution ***,the Co_(2)P nanosheets display extraordinary performance with a record high turnover frequency of 44.9 min^(-1),outperforming most of the noble-metal-free catalysts reported to *** remarkable performance is attributed to its desired nanosheets structure,featuring with high specific surface area,abundant exposed active sites,and short charge diffusion *** findings provide a novel strategy for regulating metal phosphides with desired phase structure and morphology for energy-related applications and beyond.

关键词： Ammonia borane Hydrogen generation hydrolysis Cobalt phosphide nanosheets Photocatalysis

In situ formed Mg(BH_(4))_(2) for improving hydrolysis properties of MgH_(2)

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Journal of Magnesium and Alloys 2024年第3期12卷 1204-1214页

作者： Yongyang Zhu Mili Liu liming Zeng Yin Wang Daifeng Wu Rui Li Qing Zhou Renheng Tang Fangming Xiao Institute of Resources Utilization and Rare Earth Development Guangdong Provincial Key Laboratory of Rare Earth Development and ApplicationGuangdong Academy of SciencesGuangzhou 510650China School of Materials Science and Engineering Guangdong Provincial Key Laboratory of Advanced Energy Storage MaterialsSouth China University of TechnologyGuangzhou 510641China

The hydrolysis of MgH_(2) delivers high hydrogen capacity(15.2 wt%),which is very attractive for real-time hydrogen ***,the formation of a surface passivation Mg(OH)_(2) layer and the large excess of H_(2)O required to ensure complete hydrolysis are two key challenges for the MgH_(2) hydrolysis ***,a low-cost method is reported to synthesize MgH_(2)@Mg(BH_(4))_(2) composite via ball-milling MgH_(2) with cheap and widely available B_(2)O_(3)(or B(OH)_(3)).By adding small amounts of B_(2)O_(3),the in-situ formed Mg(BH_(4))_(2) could significantly promote the hydrolysis of MgH_(2).In particular,the MgH_(2)–10 wt%B_(2)O_(3) composite releases 1330.7 mL·g^(−1) H_(2)(close to 80%theoretical hydrogen generation H_(2))in H_(2)O and 1520.4 mL·g^(−1) H_(2)(about 95%)in 0.5 M MgCl_(2) in 60 min at 26℃ with hydrolysis rate of 736.9 mL·g^(−1)·min^(−1) and 960.9 mL·g^(−1)·min^(−1) H_(2) during the first minute of the hydrolysis,*** addition,the MgCl_(2) solution allows repeated use by filtering and exhibits high cycle stability(20 cycles),therefore leading to much reduced capacity loss caused by the excess H_(2)*** show that by introducing B_(2)O_(3) and recycling the 0.5 M MgCl_(2) solution,the system hydrogen capacity can approach 5.9 wt%,providing a promising hydrogen generation scheme to supply hydrogen to the fuel cells.

关键词： hydrolysis MgH_(2) Mg(BH_(4))_(2) Hydrogen generation B_(2)O_(3) MgCl_(2)

Microscale spherical TiO_(2)powder prepared by hydrolysis of TiCl_(4)solution:Synthesis and kinetics

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Particuology 2024年第1期84卷 60-71页

作者： Peiyi Yan Ying Zhang Shili Zheng School of Rare Earths University of Science and Technology of ChinaHefei230026China Ganjiang Innovation Academy Chinese Academy of SciencesGanzhou341119China Key Laboratory of Green Process and Engineering National Engineering Research Center of Green Recycling for Strategic Metal ResourcesInstitute of Process EngineeringChinese Academy of SciencesBeijing100190China State Key Laboratory of Vanadium and Titanium Resources Comprehensive Utilization Panzhihua617000China

hydrolysis of TiCl_(4)solution is capable of preparing microscale TiO_(2)*** research studied the synthesis of microscale spherical TiO_(2)powders and the hydrolysis *** effects of the flow field generated by different agitators and baffles in the crystallizer,the initial free acid concentration,the initial equivalent TiO_(2)concentration,and the temperature on the hydrolysis progress and powder morphology were systematically *** results show that the flow field in a crystallizer can significantly affect the morphology and particle size of the powders,and the axial flow can improve the sphericity of the *** increased free HCl and equivalent TiO_(2)concentrations in the pregnant solution inhibit the forward hydrolysis reaction,prolong the time to reach equilibrium,and reduce the *** appropriate temperature matching the compositions of the pregnant solution is crucial for the powder morphology and *** with sizes ranging from around 5 um-40μm can be tuned under controlled flow field,solution compositions,and temperature *** addition,the Cheng and Wunderlich modified Avrami equation was used for the crystallization kinetic *** effects of the free HCl concentration,equivalent TiO_(2)concentration,and hydrolysis temperature are reflected in the reaction rate constant and active nuclei reduction *** the free HCl and equivalent TiO_(2)concentrations will reduce the reaction rate constant and accelerate the deactivation of the active nuclei,thus increasing the final powder size,while increasing the temperature will lead to the opposite results.

关键词： TiCl_(4) hydrolysis Microscale TiO_(2) Spherical Kinetics

Prediction model on hydrolysis kinetics of phthalate monoester:A density functional theory study

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Journal of Environmental Sciences 2024年第1期135卷 51-58页

作者： Tong Xu Jingwen Chen Deming Xia Weihao Tang Jiansheng Cui Chun Liu Shuangjiang Li College of Environmental Science and Engineering Hebei University of Science and TechnologyShijiazhuang 050000China Key Laboratory of Industrial Ecology and Environmental Engineering(Ministry of Education) School of Environmental Science and TechnologyDalian University of TechnologyDalian 116024China National-Regional Joint Engineering Research Center for Soil Pollution Control and Remediation in South China Guangdong Key Laboratory of Integrated Agro-environmental Pollution Control and ManagementInstitute of Eco-environmental and Soil SciencesGuangdong Academy of SciencesGuangzhou 510650China

As primary degradation products of phthalate esters,phthalate monoesters(MPEs)have been widely detected in various aquatic environments and drawn growing toxicological *** kinetics that is of importance for assessing environmental persistence of chemicals remain elusive for ***,kinetics of base-catalyzed and neutral hydrolysis for 18 MPEs with different leaving groups was investigated by density functional theory *** indicate that MPEs with leaving groups having p Kaofhydrolysis half-lives were calculated to vary from 3.4 min to 79.2 years(p H=7–9).A quantitative structure-activity relationship model was developed for predicting the hydrolysis kinetics *** was found that p Kaof the leaving groups and electronegativity of the MPEs are key factors determining the hydrolysis *** work may lay a theoretical foundation for better understanding the chemical process that governs MPE persistence in aquatic environments.

关键词： Phthalate monoesters Phthalate esters hydrolysis Density functional theory Quantitative structure-activity relationship

Research progress on catalysts for organic sulfur hydrolysis: Review of activity and stability

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Chinese Journal of Chemical Engineering 2024年第7期71卷 203-216页

作者： Bingning Wang Xianzhe Wang Song Yang Chao Yang Huiling Fan Ju Shangguan State Key Laboratory of Clean and Efficient Coal Utilization Taiyuan University of TechnologyTaiyuan 030024China Shanxi Engineering Center of Civil Clean Fuel Taiyuan University of TechnologyTaiyuan 030024China College of Chemical Engineering and Technology Taiyuan University of TechnologyTaiyuan 030024China College of Environmental Science and Engineering Taiyuan University of TechnologyTaiyuan 030024China

The removal of organic sulfur through catalytic hydrolysis is a significant area of research in the field of *** review provides an overview of recent advancements in catalytic hydrolysis technology of organic sulfur,including the activity,stability,and atmosphere effects of hydrolysis *** emphasis is on strategies for enhancing hydrolysis activity and anti-oxygen poisoning property of *** modification,metal doping and nitrogen doping have been found to improve the activity of *** components modification is the most commonly used method,the formation of oxygen vacancies through metal doping and creation of nitrogen basic sites through nitrogen doping also contribute to the hydrolysis of organic *** strategies for anti-oxygen poisoning are discussed in a systematic *** structural regulation of catalysts is beneficial for the desorption and diffusion of hydrogen sulfide(H_(2)S),thereby effectively inhibiting its *** doping and the addition of electronic promoters such as transition metals can protect active sites and decrease the number of active oxygen *** methods have been proven to enhance the anti-poisoning performance of ***,this article summarizes how different atmospheres affect the activity of hydrolysis *** objective of this review is to pave the way for the development of efficient,stable and widely used catalysts for organic sulfur hydrolysis.

关键词： Organic sulfur hydrolysis Catalysts Activity Stability

Generating electron spin qubit in metal-organic frameworks via spontaneous hydrolysis

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Chinese Chemical Letters 2024年第7期35卷 529-533页

作者： Xian-Fa Jiang Chongyun Shao Zhongwen Ouyang Zhao-Bo Hu Zhenxing Wang You Song State Key Laboratory of Coordination Chemistry School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China Wuhan National High Magnetic Field Center&School of Physics Huazhong University of Science and TechnologyWuhan 430074China Chaotic Matter Science Research Center Faculty of Materials Metallurgy and ChemistryJiangxi University of Science and TechnologyGanzhou 341000China Shanghai Institute of Optics and Fine Mechanics Chinese Academy of SciencesShanghai 201800China Jiangxi Provincial Key Laboratory of Functional Molecular Materials Chemistry Jiangxi University of Science and TechnologyGanzhou 341000China

Qubit,as the basic unit of quantum operations,has at least two quantum states for *** itself has no superimposable quantum states,but after injecting N atoms,the resulted nitrogenvacancy centers form excellent-performance *** the same purpose,we can also obtain qubits by modifying the matrix without effective quantum ***-1({Cu_(3)(BTC)_(2)(H_(2)O)_(3)},BTC=1,3,5-benzene-tricarboxylate)with S=0 ground state is electron paramagnetic resonance(EPR)silent,so it is not a qubit ***,the spontaneously hydrolyzed HKUST-1 produces dilute uncoupled Cu^(Ⅱ)ions with S=1/*** this paper,we utilized the hydrolysis products of HKUST-1 to obtain qubits and assembled a core-shell structural HKUST-1@ZIF-8 by ZIF-8({Zn(mim)_(2)},mim=2-methylimidazole)coated over HKUST-1 for controlling the *** experimental results clearly show that the qubits come from hydrolyzed Cu^(Ⅱ)***,the dilute uncoupled Cu^(Ⅱ)ions in this assembly can effectively reduce the decoherence of *** EPR studies show that the T_(2) of this compound is 1067 ns at 10 K.

关键词： hydrolysis Qubit Decoherent times Metal-organic framework Core-shell structure

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Erratum to:Designed imidazole-based supramolecular catalysts for accelerating oxidation/hydrolysis cascade reactions

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Nano Research 2024年第7期17卷 6773-6773页

作者： Yuanxi Liu Wenjie Xu Shichao Xu Haifeng Wu Baoli Zhang Li Song Zhen-Gang Wang State Key Laboratory of Organic-Inorganic Composites Key Lab of Biomedical Materials of Natural Macromolecules(Ministry of Education)Beijing Laboratory of Biomedical MaterialsCollege of Materials Science and EngineeringBeijing University of Chemical TechnologyBeijing 100029China National Synchrotron Radiation Laboratory CAS Center for Excellence in NanoscienceUniversity of Science and Technology of ChinaHefei 230029China

Erratum to Nano Research,2024,17(6):4916−4923 https://***/10.1007/s12274-024-6489-5 Labeling and statement of equal contribution of the authors Yuanxi Liu and Wenjie Xu were missed in the original article as well as the Electronic Supplementary *** symbols of equal contribution“§”were added to both authors in the author list,and their contribution was stated as follows:“§Yuanxi Liu and Wenjie Xu contributed equally to this work.”

关键词： hydrolysis stated statement

hydrolysis of New Transplatin Analogue Containing One Aliphatic and One Planar Heterocyclic Amine Ligand： A Density Functional Theory Study

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Chinese Journal of Chemical Physics 2008年第4期21卷 346-352页

作者： Yan Gao Li-xin Zhou Department of Chemistry Jinan University Guangzhou 510532 China

Herein we give a theoretical study of the hydrolysis processes of a novel anticancer drug trans-[PtCl2（3-pico）（ipa）] （3-pico=3-methylpyridine, ipa=isopropylamine）. Two different models, model 1 relative to isolated reactant/product （R/P, wherein R=platinum complex＋H2O, P=platinum complex＋Cl^-） and model 2 relative to reactant complex/product complex （RC/PC, wherein RC=（platinum complex）（H2O）, PC=（platinum complex）（CI^-） are employed and the geometric structures are optimized at the B3LYP level of DFT method. It is found that the processes of the reactions follow the established theory for ligand substitution in square planar complexes; the geometries of the transition states （TS） agree with the previous related work and all of the reactions are endothermic. The effects originating from the inclusion of the attacking water/released chloride into the second coordination shell of platinum in RC/PC play an important role in the thermodynamic and kinetic profiles of the reactions, that is, the barrier heights of the reactions of model 2 are increased by -26.3 and -23.8 kJ/mol for step1 and step2 respectively, and the endothermicity is considerably decreased by -420.5 and -771.2 kJ/mol compared to model 1 in the gas phase. The consideration of the bulk solvation effects increase the barrier heights for both steps of model 1 by -27.6 and -6.7 kJ/mol respectively, whereas it reduces the barrier heights by -7.9 and -29.3 kJ/mol for model 2. The reaction energies are all decreased, especially for model i, indicating more stable complexes solvated in the bulk aqueous solution than in the gas phase. Additionally, to get an accurate energy picture of the title complex, the relative free energies derived from the DFT-SCRF （density functional theory self-consistent field） calculations are compared with the relative total energies. The results are that activation energies rise for the first hydrolysis and fall for the second hydrolysis for all the systems, and for all the systems,

关键词： Trans platinum anticancer drug Density functional theory hydrolysis Aliphatic amine ligand Heterocyclic amine ligand

hydrolysis of mechanically pre-treated cellulose catalyzed by solid acid SO4^2--TiO2 in water–ethanol solvent

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Chinese Journal of Chemical Engineering 2020年第1期28卷 136-142页

作者： Xingyilong Zhang Houfang Lu Kejing Wu Yingying Liu Changjun Liu Yingming Zhu Bin Liang Institute of New Energy and Low-Carbon Technology Sichuan UniversityChengdu 610207China School of Chemical Engineering Sichuan UniversityChengdu 610065China

An efficient catalyst SO4^2--TiO2(ST) from industrial metatitanic acid has been successfully prepared to catalyze hydrolysis of ball-milling cellulose. The results show that the highest catalytic efficiency is obtained for ST calcined at 450 ℃(ST-450) with the yield of 21.8% glucose, 13.0% 5-HMF and 4.2% furfural at 200 ℃ for30 min. The ball milling of cellulose and solid acid catalyst significantly enhances the cellulose hydrolysis. The high Lewis to Bronsted acid sites ratio for ST-450 induced by bidentate ligands between SO4^2-and TiO2 benefits high organics yield, and high total acid sites contribute to the high cellulose conversion. The large pore volume of 0.29 cm^3·g^-1 and appropriate pore size of 7.35 nm of ST-450 also contribute to the high performance. High reaction temperature over 200 ℃ exhibits negative effect on glucose and 5-HMF yield due to undesired side reactions, while furfural product is stable in the reaction system. The bidentate ligands between SO4^2-and TiO2 are considered as active acid sites for cellulose hydrolysis in water–ethanol solvents.

关键词： Cellulose Industrial metatitanic acid Solid acid TiO2 hydrolysis Ball milling