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Heterostructure engineering of MoS_(2)/Mo_(2)CT_(x) nanoarray via molten salt synthesis for enhanced hydrogen evolution reaction

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Journal of Materiomics 2023年第6期9卷 1122-1128页

作者： Yanze Wu Lin Wang Zhifang Chai weiqun shi Laboratory of Nuclear Energy Chemistry Institute of High Energy PhysicsChinese Academy of SciencesBeijing100049China

Two-dimensional layered transition metal carbides(MXenes),have huge potential advantage for applications in hydrogen evolution reaction(HER).However,the hindered hydrogen evolution at large current densities and the instability of MXenes during HER remains major challenges.Herein,we report the MoS_(2)/Mo_(2)CT_(x) nanoarray with aerophobic structure via molten salt synthesis.In situ vertical distribution of MoS_(2)nanoarray on the surface of Mo_(2)CT_(x) accelerates hydrogen gas release from the electrode,exhibiting significantly enhanced catalytic activity and stability to bare MoS_(2)and Mo_(2)CT_(x).The MoS_(2)/Mo_(2)CT_(x) nanoarray possesses excellent stability at100 mA/cm^(2)for 100 h with only 3%overpotential increase.Our work provides guidance for developing high-stability MXene-based catalysts by virtue of in situ bonding between nanoarray and MXene.

关键词： Molten salt Aerophobic structure Nanoarray Hydrogen evolution reaction

A ternary mechanism for the facilitated transfer of metal ions onto metal–organic frameworks: implications for the "versatility" of these materials as solid sorbents

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Frontiers of Chemical Science and Engineering 2022年第11期16卷 1632-1642页

作者： Xiyuan Bu Ming Tian Hongqing Wang Lin Wang Liyong Yuan weiqun shi Laboratory of Nuclear Energy Chemistry Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100049China School of Chemistry and Chemical Engineering University of South ChinaHengyang 421001China

Although metal–organic frameworks offer a new platform for developing versatile sorption materials,yet coordinating the functionality,structure and component of these materials remains a great challenge.It depends on a comprehensive knowledge of a“real sorption mechanism”.Herein,a ternary mechanism for U(Ⅵ)uptake in metal–organic frameworks was reported.Analogous MIL-100s(Al,Fe,Cr)were prepared and studied for their ability to sequestrate U(Ⅵ)from aqueous solutions.As a result,MIL-100(Al)performed the best among the tested materials,and MIL-100(Cr)performed the worst.The nuclear magnetic resonance technique combined with energy-dispersive X-ray spectroscopy and zeta potential measurement reveal that U(Ⅵ)uptake in the three metal–organic frameworks involves different mechanisms.Specifically,hydrated uranyl ions form outer-sphere complexes in the surface of MIL-100s(Al,Fe)by exchanging with hydrogen ions of terminal hydroxyl groups(Al-OH_(2),Fe-OH_(2)),and/or,hydrated uranyl ions are bound directly to Al(Ⅲ)center in MIL-100(Al)through a strong inner-sphere coordination.For MIL-100(Cr),however,the U(Ⅵ)uptake is attributed to electrostatic attraction.Besides,the sorption mechanism is also pH and ionic strength dependent.The present study suggests that changing metal center of metal–organic frameworks and sorption conditions alters sorption mechanism,which helps to construct effective metal–organic frameworks-based sorbents for water purification.

关键词： U(Ⅵ) metal–organic frameworks adsorption mechanism metal node

Magnetic KIT-6 nano-composite and its amino derivatives as convenient adsorbent for U(Ⅵ)sequestration

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Frontiers of Chemical Science and Engineering 2023年第12期17卷 2037-2049页

作者： Jiafeng Ouyang Wenlu Guo Lin Wang Changming Nie Dadong Shao weiqun shi Liyong Yuan School of Environmental and Biological Engineering Nanjing University of Science and TechnologyNanjing 210094China Institute of High Energy Physics Chinese Academy of SciencesBeijing 100049China School of Chemistry and Chemical Engineering University of South ChinaHengyang 421001China

Although mesoporous silica with magnetically hybridized two-dimensional channel structures has been well studied in recent years,it remains a challenge to fabricate the counterpart with macroporous three-dimensional cubic structures since the highly acidic preparation conditions lead to dissolution of magnetic particles.Herein,we successfully prepared magnetic KIT-6 nano-composite and its amino derivatives by bearing acid-resistant iron oxide.The prepared materials exhibited excellent properties for U(VI)ions removal from aqueous solutions under various conditions.The experimental data show that the U(VI)adsorption features fast adsorption kinetics,high adsorption capacity and ideal selectivity toward U(VI).The adsorption process is of spontaneous and endothermic nature and ionic strength independence,and the adsorbents can be easily regenerated by acid treatment.Compared to pristine KIT-6,the introduction of magnetism does not reduce the efficiency of the material to remove U(VI)while exerting its role as a recovery adsorbent.The findings of this work further demonstrate the potential broad application prospects of magnetic hybrid mesoporous silica in radionuclide chelation.

关键词： magnetic nanoparticle 3D mesoporous silica amino functionalization adsorption of U(VI) acid resistance

Two tetravalent uranium silicate and germanate crystals with three membered single-ring by molten salt method:K_(2)USi_(3)O_(9)and Cs_(2)UGe_(3)O_(9)

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Chinese Chemical Letters 2022年第7期33卷 3527-3530页

作者： Xu Zhang Lei Zhang Tao Bo Shanen Huang Zhiwei Huang weiqun shi Engineering Laboratory of Advanced Energy Materials Ningbo Institute of Materials Technology and EngineeringChinese Academy of SciencesNingbo 315201China College of Nuclear Science and Technology Harbin Engineering UniversityHarbin 150001China School of Energy and Power Engineering Xi'an Jiaotong UniversityXi'an 710049China Laboratory of Nuclear Energy Chemistry Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100049China

Two tetravalent uranium silicate and germanate M_(2)U^(Ⅳ)T_(3)O_(9)(M=K,Cs;T=Si,Ge)crystals were crystalized under inert gas by molten salt flux growth method.K_(2)USi_(3)O_(9)(1)crystallizes in the monoclinic space group P1_(21)/n1 with lattice parameters a=7.1076?,b=10.4776?,c=12.2957?,γ=120°and V=915.67?^(3).Cs_(2)UGe_(3)O_(9)(2)crystallizes in a hexagonal space group P-6 with lattice constants of a=7.5138?,b=7.5138?,c=11.0114?,γ=120°and V=538.38?^(3).Bond valence calculations indicate tetravalent uranium in both structures,which contain three-membered single-ring T_(3)O_(9)^(6-) trimers.K_(2)USi_(3)O_(9) is the first uranium silicate that contains the Si_(3)O_(9)^(6-) trimers.

关键词： Uranium silicate Uranium germanate Framework Single crystal Molten salt method

Hierarchical and self-supporting honeycomb LaNi_5 alloy on nickel foam for overall water splitting in alkaline media

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Green Energy & Environment 2022年第4期7卷 799-806页

作者： Yanze Wu Yalan Liu Kui Liu Lin Wang Lei Zhang Degao Wang Zhifang Chai weiqun shi Engineering Laboratory of Advanced Energy Materials Ningbo Institute of Materials Technology and EngineeringChinese Academy of SciencesNingbo315201ZhejiangChina Laboratory of Nuclear Energy Chemistry and Key Laboratory for Biomedical Effects of Nanomaterials and Nanosafety Institute of High Energy PhysicsChinese Academy of SciencesBeijing100049China University of Chinese Academy of Sciences Beijing100049China

Ni-based metallic foams possessing large specific surfaces and open cell structures are of specific interest as catalysts or catalyst carriers for electrolysis of water.Traditional fabrication of Nickel foam limits the element modification choices to several inert transition metals only on polymer foam precursor and subsequent preparation of foam-based catalysts in aqueous solution or organic electrolyte.To expand the modification horizon,molten salt with wide electrochemical window and fast ion diffusion can achieve the reduction of highly active elements.Herein,we reported is a general and facile method to deposit directly of highly reactive element La and prepare hierarchical honeycomb LaNi_(5) alloy on Ni foam(ho-LaNi_(5)/NF).This self-supporting electrode presents excellent electrical coupling and conductivity between the Ni foam and LaNi_(5),which provides a 3D self-supported heterostructure with outstanding electrocatalytic activity and excellent durability for the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).It exhibits excellent overpotential(1.86 V)comparable to commercial coupled IrO_(2)//Pt/C(1.85 V)at a high current density of 100 m A cm^(-2).This work may pave the way for fabricating novel 3D self-supported honeycomb alloy that can be applied as electrode for usage of clean energy.

关键词： Honeycomb alloy Hierarchical structures Molten salt Hydrogen evolution reaction Oxygen evolution reaction

Temperature-responsive alkaline aqueous biphasic system for radioactive wastewater treatment

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Chinese Chemical Letters 2022年第7期33卷 3561-3564页

作者： Chuanying Liu Jianhui Lan Qibin Yan Zhipeng Wang Chao Xu weiqun shi Chengliang Xiao College of Chemical and Biological Engineering Zhejiang UniversityHangzhou 310027China Institute of Zhejiang University–Quzhou Quzhou 324000China Laboratory of Nuclear Energy Chemistry Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100049China Institute of Nuclear&New Energy Technology Tsinghua UniversityBeijing 100084China

The treatment of anionic ^(99)TcO_(4)^(-)in the waste tank with high alkalinity is still very challenging.In this work,a new temperature-responsive alkaline aqueous biphasic system(ABS)based on(tri-n–butyl)-ntetradecyl phosphonium chloride(P_(44414)Cl)was developed to remove radioactive ^(99)TcO_(4)^(-).The phase transition mechanism was studied by cloud point titration,small-angel X-ray scattering,dynamic light scattering,and molecular dynamic simulations.As the Na OH concentration or temperature increased,the P_(44414)^(+)micelle could grow and aggregate.This micelle showed a particularly high affinity toward ReO_(4)^(-)/^(99)TcO_(4)^(-)compared to other competing anions and could directly extract more than 98.6%of ^(99)TcO_(4)^(-)from simulated radioactive tank waste supernatant.Furthermore,the loaded ^(99)TcO_(4)^(-)could be easily stripped by using concentrated nitric acid rather than metal salt-based reductants.This work clearly demonstrates that the alkaline ABS is a promising separation system for solving the technetium problem in the alkaline waste tank.

关键词： Pertechnetate Ionic liquid Nuclear waste Aqueous biphasic system Sustainable chemistry

Professor Zhifang Chai:Scientific contributions and achievements

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Chinese Chemical Letters 2022年第7期33卷 3297-3302页

作者： Yuliang Zhao Chunying Chen Weiyue Feng Zhiyong Zhang Diandou Xu weiqun shi Shuao Wang Yu-Feng Li CAS Key Laboratory for Biological Effects of Nanomaterials and Nanosafety&CAS Center for Excellence in Nanoscience National Centre for Nanoscience and TechnologyBeijing 100191China CAS Key Laboratory for Biological Effects of Nanomaterials and Nanosafety&CAS-HKU Joint Laboratory of Metallomics on Health and Environment&Beijing Metallomics Facility Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100049China Division of Research and Planning Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100049China Laboratory of Nuclear Energy Chemistry Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100049China State Key Laboratory of Radiation Medicine and Protection School for Radiological and Interdisciplinary Sciences(RAD-X)and Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education InstitutionsSoochow UniversitySuzhou 215123China

Prof.Zhifang Chai,born in October 1942,is a radioanalytical chemist working at the Institute of High Energy Physics,Chinese Academy of Sciences and Soochow University.He graduated from Fudan University in 1964.As an A... 详细信息

关键词： contributions fellow graduate

Hierarchical assembly of uranyl metallacycles involving macrocyclic hosts

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Chinese Chemical Letters 2022年第7期33卷 3539-3542页

作者： Yuanyuan Liang Lei Mei Qiuyan Jin Junshan Geng Jingyang Wang Kang Liu Kongqiu Hu Jipan Yu weiqun shi Laboratory of Nuclear Energy Chemistry Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100049China University of Chinese Academy of Sciences Beijing 100049China

Actinide metallacycles are an emerging class of functional coordination assemblies,but multi-level assembly from metallacycle units toward hierarchical supramolecular structures are still rarely investigated.In this work,we put forward a novel supramolecular inclusion-based method through introducing two macrocyclic hosts,cucurbit[7]uril(CB[7])and cucurbit[8]uril(CB[8])to facilitate hierarchical assembly of uranyl metallacycles with higher complexity,and successfully prepare two different kinds of uranyl metallacycle-based complexes with intriguing hierarchical structures,a CB[7]-based four-member molecular necklace([4]MN)and a CB[8]-involved ring-in-ring supramolecular polymer chain.The results obtained here prove the feasibility of supramolecular inclusion for regulating coordination assembly of uranyl metallacycles and related hierarchical structures.It is believed that this method can be used to achieve the construction of actinide coordination assemblies with higher structural complexity.

关键词： Metallacycle Coordination self-assembly Uranyl Cucurbituril Hierarchical structure Molecular necklace

Towards understanding the correlation between UO_2^(2+) extraction and substitute groups in 2,9-diamide-1,10-phenanthroline

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Science China Chemistry 2018年第10期61卷 1285-1292页

作者： Xinrui Zhang Liyong Yuan Zhifang Chai weiqun shi Laboratory of Nuclear Energy Chemistry Institute of High Energy Physics Chinese Academy of Sciences School for Radiological and Interdisciplinary Sciences (RAD-X) and Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions Soochow University

2,9-Diamide-1,10-phenanthroline(DAPhen)ligands represent a new family of tetradentate extractants given their strong affinity to actinides and the CHON principle.Among this family,N,N′-diethyl-N,N′-ditolyl-2,9-diamide-1,10-phenanthroline(Et-TolDAPhen),initially reported by us,exhibits excellent selectivity towards actinides(U,Th,Am,Pu)over lanthanides and thus can be potentially applied in the group actinide extraction(GANEX)process for the group separation of actinides.In this article,by tailoring the lengths of alkyl chains,we synthesized other four DAPhen ligands with different substitute groups in the diamide moieties,and characterized the relationship between properties and substitute groups of DAPhen ligand.The extraction results show that three of the ligands exhibit high performance in UO_2^(2+)extraction from an acidic solution and the extracted UO_2^(2+)can be easily stripped by only using ultrapure water.Spectrophotometry titration confirms that UO_2^(2+)combined with all the four ligands in 1:1 mode.The extended X-ray absorption finestructure(EXAFS)study shows that six donor atoms comprise the first equatorial shell of the UO_2^(2+)ions bonded by the DAPhen ligands,among which two nitrogen and two oxygen atoms are from the DAPhen ligand,while other two oxygen atoms are from one nitrate ions.This article promises to provide basic data for assessing the feasibility of this kind of DAPhen ligands applied in actinides separation from nuclear wastes.

关键词：抽取 UO2 代用品关联组织家庭提炼罐头