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Unlocking single-atom catalysts via amorphous substrates

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Nano research 2024年第5期17卷 3533-3546页

作者： Bohua Sun Mingyuan Xu Xiaoxia Li Baohong Zhang Rui Hao Xiaoyu Fan Binbin Jia Dingshun She School of engineering and Technology China University of Geosciences(Beijing)Beijing 100083China Zhengzhou Institute China University of Geosciences(Beijing)Zhengzhou 451283China College of materials and Chemical engineering Key Laboratory of Inorganic Nonmetallic Crystalline and Energy Conversion MaterialsChina Three Gorges UniversityYichang 443002China School of Chemistry Beihang UniversityBeijing 100191China Chinese Academy of Sciences(CAS)Key Laboratory of Nanosystem and Hierarchy Fabrication CAS Center for Excellence in NanoscienceNational Center for Nanoscience and TechnologyBeijing 100190China national engineering research center of nonferrous metals Materials and Products for New EnergyChina GRINM Group Co.Ltd.Beijing 100088China

Single-atom catalysts(SACs)reveal great potential for application in catalysis due to their fully exposed active sites.In general,single atoms(SAs)and the coordination substrates need to have strong interactions or charge transfer to ensure the atomic dispersion,which requires the selection of a suitable substrate to stabilize the target atoms.Recent studies have demonstrated that amorphous materials with abundant defects and coordinatively unsaturated sites can be used as substrates for more efficient capturing SAs,further enhancing the catalytic performance.In this review,we discuss recent research progress of SAs loaded on amorphous substrates for enhanced catalytic activity.Firstly,we summarize the commonly used amorphous substrates for stabilizing SAs.Subsequently,we present several advanced applications of amorphous SACs in the field of catalysis,including electrocatalysis and photocatalysis.And then,we also clarify the synergistic mechanism between SAs and amorphous substrate on catalytic process.Finally,we summarize the challenges with our personal views and provide a critical outlook on how amorphous SACs continue to evolve.

关键词： single-atoms amorphous substrate synthetic strategy catalysis

Heterostructure:application of absorption-catalytic center in lithium-sulfur batteries

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Rare metals 2024年第4期43卷 1461-1487页

作者： Fei Wang Chun-Man Yang Yong-Qi Wang Dan You Wen-Hao Yang Rong-Wei Huang Ji-Yue Hou Qian Wang Ying-Jie Zhang Ying Wang Yue-Jing Zeng Yi-Yong Zhang Xue Li national Local Joint engineering research center for Lithium-Ion Batteries and materials Preparation Technology Key Laboratory of Advanced Batteries Materials of Yunnan ProvinceFaculty of Metallurgical and Energy Engineering Kunming University of Science and Technology College of Electrical Information engineering Panzhihua University State Key Laboratory of Physical Chemistry of Solid Surfaces Collaborative Innovation Centre of Chemistry for Energy MaterialsState-Province Joint Engineering Laboratory of Power Source Technology for New Energy VehicleEngineering Research Center of Electrochemical TechnologyMinistry of EducationCollege of Chemistry and Chemical Engineering Xiamen University

Due to the high theoretical specific capacity(1675 mAh·g-1),low cost,and high safety of the sulfur cathodes,they are expected to be one of the most promising rivals for a new generation of energy storage systems.However,the shuttle effect,low conductivity of sulfur and its discharge products,volume expansion,and other factors hinder the commercialization of lithium-sulfur batteries（LSBs）.The development of sulfur-fixing materials and the design of multifunctional materials to enhance the electrochemical performance of LSBs have been the main research priorities in recent years.Because of the advantages of high conductivity,built-in electric field,and good synergism,more and more researchers have employed heterostructure into sulfur-fixing materials to enhance the catalytic and absorption ability for polysulfides.In this review,the principle of heterostructure and the mechanism of enhancing the performance of lithium-sulfur batteries are described.The applications of heterostructure in cathode and interlayer of LSBs in the latest years are summarized.Finally,the cutting-edge troubles and possibilities of heterostructures in LSBs are briefly presented.

关键词： Lithium–sulfur batteries (LSBs) Heterostructure Built-in electric field Catalytic Absorption

Multidimensional regulation of Ti-Zr-Cr-Mn hydrogen storage alloys via Y partial substitution

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Nano research 2024年第5期17卷 4211-4220页

作者： Haixiang Xiu Wanqiang Liu Dongming Yin Nan Ding Wenfeng Qiao Shaolei Zhao Long Liang Cong Liu Shaohua Wang Qingshuang Wang Bingbing Chen Limin Wang Yong Cheng School of materials Science and engineering Changchun University of Science and TechnologyChangchun 130022China State Key Laboratory of Rare Earth Resources Utilization Changchun Institute of Applied ChemistryChinese Academy of Sciences(CAS)Changchun 130022China School of Applied Chemistry and engineering University of Science and Technology of ChinaHefei 230026China Department of energy Science and engineering Nanjing Tech UniversityNanjing 211816China national engineering research center of nonferrous metals materials and products for new energy GRINM Group Co.Ltd.Beijing 100088China GRIMAT engineering Institute Co. Ltd.Beijing 101407China College of Life Science and Technology Changchun University of Science and TechnologyChangchun 130022China

High density and safe storage of hydrogen are the preconditions for the large-scale application of hydrogen energy.Herein,the hydrogen storage properties of Ti_(0.6)Zr_(0.4)Cr_(0.6)Mn_(1.4) alloys are systematically studied by introducing Y element instead of Ti element through vacuum arc melting.After the partial substitution of Y,a second phase of rare earth oxide is added in addition to the main suction hydrogen phase,C14 Laves phase.Thanks to the unique properties of rare earth elements,the partial substitution of Y can not only improve the activation properties and plateau pressure of the alloys,but also increase the effective hydrogen storage capacity of the alloys.The comprehensive properties of hydrogen storage alloys are improved by multidimensional regulation of rare earth elements.Among them,Ti_(0.552)Y_(0.048)Zr_(0.4)Cr_(0.6)Mn_(1.4) has the best comprehensive performance.The alloy can absorb hydrogen without activation at room temperature and 5 MPa,with a maximum hydrogen storage capacity of 1.98 wt.%.At the same time,it reduces the stability of the hydride and the enthalpy change value,making it easier to release hydrogen.Through theoretical analysis and first-principle simulation,the results show that the substitution of Y element reduces the migration energy barrier of hydrogen and the structural stability of the system,which is conducive to hydrogen evolution.The alloy has superior durability compared to the original alloy,and the capacity retention rate was 96.79%after 100 hydrogen absorption/desorption cycles.

关键词： AB_(2)-type hydrogen storage alloy rare earth element first-principles simulation multidimensional regulation

Atomistic mechanism of high ionic conductivity in lithium ytterbium-based halide solid electrolytes:A first-principles study

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Journal of Rare Earths 2024年第1期42卷 155-162,I0006页

作者： Limin Wang Wei Xiao Lu Sun Rong Yang Jinqiu Yu Ligen Wang State Key Laboratory of nonferrous metals and Processes China GRINM Group Co.Ltd.Beijing100088China GRIMAT engineering Institute Co. Ltd.Beijing101407China General research Institute for nonferrous metals Beijing100088China China Automotive Battery research Institute Co. Ltd.Beijing101407China Rare Earth Functional materials(Xiong'an)Innovation center Co. Ltd.Xiong'an071700China

As the next generation of commercial automotive power batteries begins replacing liquid lithium batteries,many look towards all-solid-state batteries to pioneer the future.All-so lid-state batteries have attracted the attention of countless researchers around the world because of their high safety and high energy density.In recent times,halide solid-state electrolytes have become a research hotspot within solid-state electrolytes because of their potentially superior properties.In this paper,in the framework of DFT,we investigated the atomic mechanisms of improving the ionic conductivity and stability of Li_(3)YbCl_(6).Our calculations show that both trigonal and orthorhombic Li_(3)YbCl_(6) exhibit wide electrochemical windows and metastable properties(100 meV/atom>Ehull>0 meV/atom).However,the orthorhombic Li_(3)YbCl_(6) can be stabilized at high temperatures by taking the vibrational entropy into account,which is supported by the experimental results.Moreover,it is expected that because of the Yb/Li synergistic interactions that,due to their strong mutual coulomb repulsion,influence the Li^(+)transport behavior,the orthorhombic Li_(3)YbCl_(6) might have superior ionic conductivities with appropriate Li+migration paths determined by the Yb^(3+) distribution.Also,higher ionic conductivities can be obtained by regulating the random distribution of Li^(+) ions.Further Li^(+)-deficiency can also largely increase the ionic conductivity by invoking vacancies.This study helps gain a deeper understanding of the laws that govern ionic conductivities and stabilities and provides a certain theoretical reference for the experimental development and design of halide solid-state electrolytes.

关键词： Halide solid-state electrolytes Phase stability Ionic conductivity First-principles calculations Rare earths

The energy response of LaBr_(3)(Ce),LaBr_(3)(Ce,Sr),and NaI(Tl)crystals for GECAM

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Nuclear Science and Techniques 2024年第2期35卷 110-122页

作者： Pei-Yi Feng Xi-Lei Sun Zheng-Hua An Yong Deng Cheng-Er Wang Huang Jiang Jun-Jie Li Da-Li Zhang Xin-Qiao Li Shao-Lin Xiong Chao Zheng Ke Gong Sheng Yang Xiao-Jing Liu Min Gao Xiang-Yang Wen Ya-Qing liu Yan-Bing Xu Xiao-Yun Zhao Jia-Cong Liu Fan Zhang Hong Lu Particle and Astrophysics center Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100049China Key Laboratory of Particle Astrophysics Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100049China University of Chinese Academy of Sciences Chinese Academy of SciencesBeijing 100049China Experimental Physics center Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100049China State Key Laboratory of Particle Detection and Electronics Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100049China School of Nuclear Science and Technology University of South ChinaHengyang 421001China national engineering research center for Rare Earth Grirem Advanced Materials Co.Ltd.and General Research Institute for Nonferrous MetalsBeijing 100088China

The GECAM series of satellites utilizes LaBr_(3)(Ce),LaBr_(3)(Ce,Sr),and NaI(Tl)crystals as sensitive materials for gamma-ray detectors(GRDs).To investigate the nonlinearity in the detection of low-energy gamma rays and address the errors in the calibration of the E-C relationship,comprehensive tests and comparative studies of the three aforementioned crystals were conducted using Compton electrons,radioactive sources,and mono-energetic X-rays.The nonlinearity test results of the Compton electrons and X-rays demonstrated substantial differences,with all three crystals presenting a higher nonlinearity for X/-rays than for Compton electrons.Despite the LaBr_(3)(Ce)and LaBr_(3)(Ce,Sr)crystals having higher absolute light yields,they exhibited a noticeable nonlinear decrease in the light yield,especially at energies below 400 keV.The NaI(Tl)crystal demonstrated an"excess"light output in the 6-200 keV range,reaching a maximum"excess"of 9.2%at 30 keV in the X-ray testing and up to 15.5%at 14 keV during Compton electron testing,indicating a significant advantage in the detection of low-energy gamma rays.Furthermore,we explored the underlying causes of the observed nonlinearity in these crystals.This study not only elucidates the detector responses of GECAM,but also initiates a comprehensive investigation of the nonlinearity of domestically produced lanthanum bromide and sodium iodide crystals.

关键词： LaBr_(3)(Ce)detector LaBr_(3)(Ce,Sr)detector NaI(Tl)detector GECAM energy response Light yield nonlinearity

Plume-lithosphere interaction in the Comei Large Igneous Province: Evidence from two types of mafic dykes in Gyangze, south Tibet, China

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China Geology 2024年第1期7卷 80-90页

作者： Ya-ying Wang Ling-sen Zeng Li-e Gao Li-long Yan Ling-hao Zhao Jia-hao Gao Ying-long Di Guang-xu Li Yi-hong Tian Institute of Geology Chinese Academy of Geological SciencesBeijing 100037China national research center for Geoanalysis Chinese Academy of Geological SciencesBeijing 100037China China nonferrous metals(Guilin)Geology and Mining Co. LtdGuilin 541004China

Two suites of mafic dykes,T1193-A and T1194-A,outcrop in Gyangze area,southeast Tibet.They are in the area of Comei LIP and have indistinguishable field occurrences with two other dykes in Gyangze,T0902 dyke with 137.7±1.3 Ma zircon age and T0907 dyke with 142±1.4 Ma zircon age reported by Wang YY et al.(2016),indicating coeval formation time.Taking all the four diabase dykes into consideration,two different types,OIB-type and weak enriched-type,can be summarized.The“OIB-type”samples,including T1193-A and T0907 dykes,show OIB-like geochemical features and have initial Sr-Nd isotopic values similar with most mafic products in Comei Large Igneous Provinces(LIP),suggesting that they represent melts directly generated from the Kerguelen mantle plume.The“weak enriched-type”samples,including T1194-A and T0902 dykes,have REEs and trace element patterns showing withinplate affinity but have obvious Nb-Ta-Ti negative anomalies.They show uniform lowerεNd(t)values(−6‒−2)and higher 87Sr/86Sr(t)values(0.706‒0.709)independent of their MgO variation,indicating one enriched mantle source.Considering their closely spatial and temporal relationship with the widespread Comei LIP magmatic products in Tethyan Himalaya,these“weak enriched-type”samples are consistent with mixing of melts from mantle plume and the above ancient Tethyan Himalaya subcontinental lithospheric mantle(SCLM)in different proportions.These weak enriched mafic rocks in Comei LIP form one special rock group and most likely suggest large scale hot mantle plume-continental lithosphere interaction.This process may lead to strong modification of the Tethyan Himalaya lithosphere in the Early Cretaceous.

关键词： OIB type diabase Comei Large Igneous Province Weakly enriched diabase Plume-lithosphere interaction Nb-Ta-Ti negative anomaly Kerguelen plume Geological survey engineering Tibet Plateau

Orientation controlled photogenerated carriers on selfsupporting CdS/Ni3S2 paper toward photocatalytic hydrogen evolution and biomass upgrading

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Rare metals 2024年第5期43卷 2015-2025页

作者： Xiao-Yan Liu Qing Cao Gui-Xiang Li Hui Liu Li-Li Zeng Li-Li Zhao Bin Chang Xi-Wen Wang Hong Liu Wei-Jia Zhou Institute for Advanced Interdisciplinary research School of Chemistry and Chemical Engineering University of Jinan Institute of Chemistry and Biochemistry Freie Universit?t Berlin Institute of Chemical Sciences and engineering école Polytechnique Fédérale de Lausanne KAUST Catalysis center King Abdullah University of Science and Technology Thuwal 23955-6900 School of Environment and energy South China University of TechnologyGuangzhou Higher Education Mega Center State Key Laboratory of Crystal materials Shandong University School of Mechanical engineering Xi'an Jiaotong University

The appropriate regulation of band structure is an effective strategy in constructing efficient photocatalytic systems.Present photocatalytic system mainly employs powder photocatalysts,which makes their recovery reliant on expensive separation processes and severely limits their industrial application.Herein,we constructed a novel Cd S/Ni3S2heterostructure using free-standing and flexible nickel fiber paper as the matrix.The regulated energy band structure achieves effective electron–hole separation.The as-synthesized flexible photocatalyst exhibits considerable photocatalytic activity toward the H2evolution reaction under visible-light irradiation,with an H2production rate of5.63μmol·cm-2·h-1(14.1 mmol·g-1cat·h-1according to the catalyst loading content).Additionally,the otherwisewasted excited holes simultaneously drive organic transformations to yield value-added organic products,thus markedly improving the photocatalytic H2evolution rate.Such a photocatalytic system is scaled up further,where a self-supported 20 cm×25 cm sample achieves a champion H2production rate of 60–80μmol·h-1under practical sun irradiation.This newly developed self-supported photocatalyst produces opportunities for practical solar H2production with biomass upgrading.

关键词： Self-supporting photocatalyst CdS/Ni 3 S 2 heterojunction Hydrogen evolution Biomass upgrading Large-scale application

Stabilization/solidification mechanisms of tin tailings and fuming slag-based geopolymers for different heavy metals

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Frontiers of Environmental Science & engineering 2024年第5期18卷 43-55页

作者： Xian Zhou Zhengfu Zhang Hui Yang School of materials Science and engineering Kunming University of Science and TechnologyKunming650093China Kunming Metallurgical research Institute Co. Ltd.Kunming650031China

Tin mine tailings(TMT)and fuming slag(FS)contain many heavy metals(As,Cr,Cu,Zn and Mn)that cause severe pollution to the environment.Herein,geopolymers were prepared using TMT,FS and flue gas desulfurization gypsum(FGDG)to immobilize heavy metals,and their compressive strength and heavy metal leaching toxicity were investigated.It was first determined that T4F5(TMT:FS=4:5)sample exhibited the highest compressive strength(7.83 MPa).T4F5 achieved 95%immobilization efficiency for As and Cr,and nearly 100%for Cu,Zn and Mn,showing good immobilization performance.A series of characterization analyses showed that heavy metal cations can balance the charge in the geopolymer and replace Al in the geopolymer structure to form covalent bonds.In addition,about 2%–20%of heavy metal Fe was immobilized in hydration products,heavy metal hydroxides and non-bridging Si–O and Al–O coordination with silica-aluminate matrices.AsO33−was oxidized into AsO43−,which may form Ca–As or Fe–As precipitates.Cr2O72−was converted to CrO42−under alkaline environment and then combined with OH−to form Cr(OH)3 precipitates.Mn2+may react directly with dissolved silicate to form Mn2SiO4 and also form Mn(OH)2 precipitates.The unstable Mn(OH)2 can be further oxidized to MnO2.The heavy metal cations were immobilized in the silicoaluminate lattice,while the anions tended to form insoluble precipitates.These results may benefit the industry and government for better handling of TMT,FS and solid wastes containing the abovementioned five heavy metals.

关键词： Heavy metals Cementitious materials Tin tailings Stabilization/solidification Redox

Oxidation behavior of Al0.2CoCrFeNi high-entropy alloy film in supercritical water environment

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Rare metals 2022年第4期41卷 1217-1222页

作者： Bao-Hong Zhu Hao-Chen Qiu Wei Jiang Qing-He Yu GRIMAT engineering Institute Co. LtdBeijing 101407China General research Institute for nonferrous metals Beijing 100088China national engineering research center of nonferrous metals materials and products for new energy GRINM Group Co.Ltd.Beijing 100088China

The corrosion resistance of Al0.2CoCrFeNi high-entropy alloy(HEA) film deposited by magnetron sputtering was investigated and compared with that of Al0.2 CoCrFeNi HEA bulk and G115 alloy.The HEA film is composed of face-centered cubic with nanoscale grain size.The HE As(film and bulk) exhibit higher electro-chemical corrosion resistance than the G115 alloy in 3.5 wt% NaCl solution.

关键词： alloy corrosion resistance