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Journal of Environmental Sciences 2024年第2期136卷 390-399页

作者： Aihua Cheng Yi He xiaohe liu Chi He Department of Environmental Engineering College of Geology and EnvironmentXi’an University of Science and TechnologyXi’an 710054China State Key Laboratory of Multiphase Flow in Power Engineering School of Energy and Power EngineeringXi’an Jiaotong UniversityXi’an 710049China National Engineering Laboratory for VOCs Pollution Control Material and Technology University of Chinese Academy of SciencesBeijing 101408China

Achieving an efficient and stable heterogeneous Fenton reaction over a wide pH range is of great significance for wastewater treatment.Here,a pollen-derived biochar catalyst with a unique honeycomb-like structure,coupled with the dispersion of magnetic Fe_(3)O_(4)/FeS(Fe/S)nanoparticles,was synthesized by simple impregnation precursor,followed by pyrolysis.The prepared Fe/S-biochar catalyst demonstrated outstanding phenol degradation efficiency across a wide pH range,with 98%of which eliminated even under neutral conditions(pH 7.0).The high catalytic activity was due to the multilevel porous structure of pollenderived biochar provided enough active sites and allowed for better electron transfer,then increases oxidation ability to promote the reaction.Moreover,the acid microenvironment formed by SO_(4)^(2-)group from Fe/S composite extended the pH range for Fenton reaction,and S^(2-)facilitated the conversion of≡Fe^(3+)to≡Fe^(2+),resulting in remarkable degradation efficiency.Further,biochar can effectively promote cycling stability by limiting Fe leaching.This work may provide a general strategy for designing 3D framework biochar-based Fe/S catalysts with excellent performance for heterogeneous Fenton reactions.

关键词： Biomass Biochar Fenton reaction Fe_(3)O_(4)/FeS(Fe/S) Phenol degradation

Boosting charge transfer via interface charge reconstruction between amorphous NiFe-LDH and crystalline NiCo_(2)O_(4)for efficient alkaline water/seawater oxidation

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Nano Research 2024年第6期17卷 4856-4863页

作者： Zhonghang Xing Yi Zhao Yunhai Wang xiaohe liu Zhiqiang Guo Qingyun Chen International Research Center for Renewable Energy and State Key Laboratory of Multiphase Flow in Power Engineering Xi’an Jiaotong UniversityXi’an 710049China Department of Environmental Science and Engineering Xi’an Jiaotong UniversityXi’an 710049China China School of Geology and Environment Xi’an University of Science and TechnologyXi’an 710049China Changqing Engineering Design Co. Ltd.Xi’an 710018China

Electrocatalysts with optimal efficiency and durability for the oxygen evolution reaction(OER)are becoming increasingly important as the demand for alkaline water/seawater electrolysis technology grows.Herein,a novel rose-shaped NiFe-layered double hydroxide(LDH)/NiCo_(2)O_(4)composed of amorphous wrinkled NiFe-LDH and highly crystalline NiCo_(2)O_(4)was synthesized with rich heterointerfaces.Many unsaturated metal sites are generated due to significant charge reconstruction at the heterointerface between the crystalline and amorphous phases.These metal sites could trigger and provide more active sites.The density functional theory(DFT)reveals that a new charge transfer channel(Co-Fe)was formed at the heterointerface between NiFe-LDH as electron acceptor and NiCo_(2)O_(4)as electron donor.The new charge transfer channel boosts interfacial charge transfer and enhances catalytic efficiency.The NiFe-LDH/NiCo_(2)O_(4)/nickel foam(NF)drives current densities of 10 and 100 mA·cm−2 with overpotentials of 193 and 236 mV,respectively.The composite electrode demonstrates a fast turnover frequency(0.0143 s−1)at 1.45 V vs.RHE(RHE=reversible hydrogen electrode),which is 5.5 times greater than pure NiCo_(2)O_(4),suggesting its superior intrinsic activity.Additionally,NiFe-LDH/NiCo_(2)O_(4)/NF electrode exhibited negligible degradation after 150 h of uninterrupted running in alkaline seawater oxidation.This study introduces a method for preparing high-efficiency electrocatalysts utilized in alkaline water/seawater electrolysis.

关键词： NiFe-layered double hydroxide(LDH)/NiCo_(2)O_(4)/nickel foam(NF) heterogeneous interfaces charge reconstruction water/seawater electrolysis

Recent advances in multifunctional metal-organic frameworks for lithium metal batteries

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Science China Chemistry 2024年第3期67卷 759-773页

作者： Jiaqi Li Zheng Weng Zuosu Qin Ying Zhang Ning Zhang xiaohe liu Chuankun Jia Gen Chen Jiang Zhou School of Materials Science and Engineering Key Laboratory of Electronic Packaging and Advanced Functional Materials of Hunan ProvinceCentral South University Zhongyuan Critical Metals Laboratory Zhengzhou University College of Materials Science and Engineering Changsha University of Science&Technology

In view of novel materials in the field of lithium metal batteries(LMBs), metal-organic frameworks(MOFs) have attracted extensive research interest owing to their controllable pore size, unsaturated metal sites and multifunctional organic groups. A variety of MOFs have been elaborately calculated and synthesized to be applied as separator coating, electrolyte modulators and solid-state electrolyte fillers in LMBs. In this mini-review, we summarize the mechanism of MOFs to limit the migration of anions, improve the Li-ion transference number and prolong the lifespan of LMBs. Suitable pore structure of MOFs can physically restrict the movement of Li^(+). Unsaturated metal sites can adsorb anions by electrostatic interaction. In addition,multifunctional organic functional groups that limit the migration of anions are discussed. Finally, the key challenges and perspectives in the development direction of MOFs-based separators and electrolytes are further elaborated.

关键词： metal-organic frameworks lithium metal battery separator electrolyte

Contact engineering for temperature stability improvement of Bi-contacted MoS2 field effect transistors

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Science China(Information Sciences) 2024年第6期67卷 172-179页

作者： Zizheng liu Qing ZHANG xiaohe HUANG Chunsen liu Peng ZHOU State Key Laboratory of Integrated Chip and Systems School of MicroelectronicsZhangjiang Fudan International Innovation CenterFudan University Frontier Institute of Chip and System Shanghai Key Lab for Future Computing Hardware and SystemFudan University Shaoxin Laboratory

Semimetallic bismuth（Bi） is one of the most effective strategies for reducing the contact resistance of two-dimensional transition metal dichalcogenide field effect transistors（FETs）. However, the low melting point of Bi contact（271.5℃） limits its reliable applications. In this study, we demonstrated that the temperature stability of Bi-contacted electrodes could be improved by inserting a high-melting point semimetallic antimony（Sb） between the Bi contacting layer and the gold（Au） capping layer. The proposed Bi/Sb/Au contact electrodes tended to form a metal mixture with a continuous surface during the heating process（Voids appeared on the surface of the Bi/Au contact electrodes after heating at 120℃）. Because of the improved contacting layer formed by the semimetal Bi/Sb alloy, the fabricated Bi/Sb/Au-contacted molybdenum sulfide（MoS2） FETs with different gate lengths demonstrated higher on-state current stability after heating treatment than the Bi/Au contact. Because of the Bi/Sb/Au contact and poly（methyl methacrylate） package, the MoS2FETs demonstrated time stability of at least two months from the almost unchanged transfer characteristics. The electrical stability indicates that the insertion of semimetallic Sb is a promising technology for reliable Bi-based contact.

关键词： temperature stability semimetallic bismuth contact semimetallic antimony contact MoS$_{2}$ FETs time stability

Advanced silicon nanostructures derived from natural silicate minerals for energy storage and conversion

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Green Energy & Environment 2022年第2期7卷 205-220页

作者： Hao Wan Wei Ma Kechao Zhou Yijun Cao xiaohe liu Renzhi Ma School of Chemical Engineering Zhengzhou UniversityZhengzhou450001China State Key Laboratory of Powder Metallurgy Central South UniversityChangsha410083China International Center for Materials Nanoarchitectonics(WPI-MANA) National Institute for Materials Science(NIMS)Namiki 1-1TsukubaIbaraki305-0044Japan

To effectively alleviate the ever-increasing energy crisis and environmental issues,clean and sustainable energy-related materials as well as the corresponding storage/conversion devices are in urgent demand.Silicon(Si) with the second most elemental abundance on the crust in the form of silicate or silica(SiO_(2)) minerals,is an advanced emerging material showing high performance in energy-related fields(e.***.batteries,photocatalytic hydrogen evolution).For the improved performance in industry-scale applications,Si materials with delicate nanostructures and ideal compositions in a massive production are highly cherished.On account of the reserve,low cost and diverse micro-nanostructures,silicate minerals are proposed as promising raw materials.In the article,crystal structures and the reduction approaches for silicate minerals,as well as recent progress on the as-reduced Si products for clean energy storage/conversion,are presented systematically.Moreover,some cutting-edge fields involving Si materials are discussed,which may offer deep insights into the rational design of advanced Si nanostructures for extended energy-related fields.

关键词： minerals massive silicate

Engineering d-band states of(CuGa)_(x)Zn_(1-2x)Ga_(2)S_(4)material for photocatalytic syngas production

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Journal of Energy Chemistry 2023年第4期79卷 365-372页

作者： Peng liu Baopeng Yang Ziyi Xiao Shengyao Wang Shimiao Wu Min liu Gen Chen xiaohe liu Renzhi Ma Ning Zhang School of Materials Science and Engineering Central South UniversityChangsha 410083HunanChina School of Physical Science and Electronics Central South UniversityChangsha 410083HunanChina College of Science Huazhong Agricultural UniversityWuhan 430070HubeiChina School of Chemical Engineering Zhengzhou UniversityZhengzhou 450001HenanChina International Center for Materials Nanoarchitectonics(MANA) National Institute for Materials Science(NIMS)1-1 NamikiTsukubaIbaraki 305-0044Japan

The d-band states of catalytic materials participate in adsorbing reactive intermediate species and determine the catalytic behaviors in CO_(2)reduction reactions.However,surface d-band states relating to the photocatalytic CO_(2)reduction reactions behaviors are rarely concerned.Herein,a slightly amount of Cd^(2+)is decorated on the surface of(CuGa)_(x)Zn_(1-2x)Ga_(2)S_(4)material(Cd^(2+)/(CuGa)_(x)Zn_(1-2x)Ga_(2)S_(4))to tune the surface d-band states for improved CO_(2)+2reduction reactions.The Cd/(CuGa)_(x)Zn_(1-2x)Ga_(2)S_(4)is fabricated via the facile ions-exchange method to make that slightly Zn2+is substituted by Cd^(2+).The Cd^(2+)/(CuGa)_(x)Zn_(1-2x)Ga_(2)S_(4)exhibits much enhanced photocatalytic activity in CO_(2)reduction reactions to produce CO and water splitting to produce H_(2).Physical characterizations show that the energy band structure is not changed obviously.Density functional theory reveals that Cd^(2+)/(CuGa)_(x)Zn_(1-2x)Ga_(2)S_(4)possesses a closer shift of d-band center to Fermi level than(CuGa)_(x)Zn_(1-2x)Ga_(2)S_(4),suggesting easier adsorption of CO_(2)reduction reactive intermediates after Cd^(2+)decoration.Further calculations confirm that a relatively reduced adsorption Gibbs energy of reactive intermediates in CO_(2)reduction reaction is required on Zn atoms in Cd^(2+)/(CuGa)_(x)Zn_(1-2x)Ga_(2)S_(4)material,benefiting the photocatalytic CO_(2)reduction reactions.This work engineers surface d-band states by surface Cd^(2+)decoration,which gives an effective strategy to design highly efficient photocatalysts for syngas production.

关键词： Photocatalysisd-band state Density functional theory Sulfide semiconductor Surface modification

Microcrystallization and lattice contraction of NiFe LDHs for enhancing water electrocatalytic oxidation

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Carbon Energy 2022年第5期4卷 901-913页

作者： Zhicheng Zheng Dan Wu Gen Chen Ning Zhang Hao Wan xiaohe liu Renzhi Ma State Key Laboratory of Powder Metallurgy School of Materials Science and EngineeringCentral South UniversityChangshaHunanPR China School of Chemical Engineering Zhengzhou UniversityZhengzhouHenanPR China International Center for Materials Nanoarchitectonics(WPI-MANA) National Institute for Materials Science(NIMS)IbarakiJapan

The lattice-oxygen-mediated mechanism is considered as a reasonable mechanism for the electrochemical catalytic oxygen evolution reaction(OER)of NiFe layered double hydroxides(LDHs).A NiFe LDH with distinct lattice contraction and microcrystallization was synthesized via a simple one-step method using sodium gluconate.The lattice contraction is attributed to the interaction of carbon in sodium gluconate and iron in NiFe LDH.The NiFe LDH with optimized microcrystallization and lattice contraction shows a low overpotential of 217 mV at a current density of 10 mA cm^(−2) and excellent durability of 20 h at a high current density of 100 mA cm^(−2).The results revealed that a contractive metal–oxygen bond could boost the intrinsic activity of active sites and the microcrystallization promotes an increase in the number of active sites in terms of unit area.The chemical environment of oxygen elemental characterization and resistance at different chronopotentiometry times confirm that the lattice oxygen element is indeed involved in the process of OER,supporting the lattice-oxygen-mediated mechanism of NiFe LDH.Density functional theory calculations reveal that contractive metal–oxygen bonds induced a reduction of the adsorption energy barrier of intermediate products,thus improving the intrinsic catalytic activity.The special characteristics of microcrystallization and lattice contraction of NiFe LDH provide a strategy to improve both the number and the intrinsic activity of active sites in a versatile manner.

关键词： lattice contraction lattice-oxygen-mediated mechanism microcrystallization NiFe LDH oxygen evolution reaction

Tuned d-band states over lanthanum doped nickel oxide for efficient oxygen evolution reaction

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Nano Materials Science 2023年第2期5卷 228-236页

作者： Ziyi Xiao Wei Zhou Baopeng Yang Chengan Liao Qing Kang Gen Chen Min liu xiaohe liu Renzhi Ma Ning Zhang School of Materials Science and Engineering Central South UniversityChangsha410083HunanChina Department of Applied Physics Tianjin Key Laboratory of Low Dimensional Materials Physics and Preparing TechnologySchool of ScienceTianjin UniversityTianjin300072China School of Physical Science and Electronics Central South UniversityChangsha410083HunanChina Institute of Surface Analysis and Chemical Biology University of JinanJinan250022ShandongChina International Center for Materials Nanoarchitectonics(MANA) National Institute for Materials Science(NIMS)1-1 NamikiTsukubaIbaraki305-0044Japan

The d-band state of materials is an important descriptor for activity of oxygen evolution reaction(OER).For NiO materials,there is rarely concern about tuning their d-band states to tailor the OER behaviors.Herein,NiO nanocrystals with doping small amount of La^(3+)were used to regulate d-band states for promoting OER activity.Density of states calculations based on density functional theory revealed that La^(3+)doping produced upper shift of d-band center,which would induce stronger electronic interaction between surface Ni atoms and species of oxygen evolution reaction intermediates.Further density functional theory calculation illustrated that La^(3+)doped NiO possessed reduced Gibbs free energy in adsorbing species of OER intermediate.Predicted by theoretical calculations,trace La^(3+)was introduced into crystal lattice of NiO nanoparticles.The La^(3+)doped NiO nanocrystal showed much promoted OER activity than corresponding pristine NiO product.Further electrochemical analysis revealed that La^(3+)doping into NiO increased the intrinsic activity such as improved active sites and reduced charge transfer resistance.The in-situ Raman spectra suggested that NiO phase in La^(3+)doped NiO could be better maintained than pristine NiO during the OER.This work provides an effective strategy to tune the d-band center of NiO for efficient electrocatalytic OER.

关键词： Nickel oxide Oxygen evolution reaction D-band center Electrocatalysis Water splitting

Anchoring Active Sites by Pt_(2)FeNi Alloy Nanoparticles on NiFe Layered Double Hydroxides for Efficient Electrocatalytic Oxygen Evolution Reaction

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Energy & Environmental Materials 2022年第1期5卷 270-277页

作者： Zhicheng Zheng Yanru Guo Hao Wan Gen Chen Ning Zhang Wei Ma xiaohe liu Shuquan Liang Renzhi Ma School of Materials Science and Engineering Central South University College of Chemistry and Molecular Engineering Peking University School of Chemical Engineering Zhengzhou University International Center for Materials Nanoarchitectonics (WPI-MANA) National Institute for Materials Science (NIMS)

Strategy of anchoring alloy nanoparticles made up of the efficient catalytic element(e.g.,Ni,Fe)on dodecyl sulfate(DS^(-))-intercalated NiFe layered double hydroxides(DS^(-)-NiFe LDH)obtained by a convenient one-step hydrothermal coprecipitation method for essentially enhancing oxygen evolution reaction(OER)performance was proposed.The results of structural characterization indicate Pt_(2)FeNi alloy nanoparticles evenly distribute on the surface of DS^(-)-NiFe LDH.The sizes of the Pt_(2)FeNi nanoparticles,closely related to their OER performance,could be wellcontrolled by adjusting the amount of H;PtCl;addition.The composite structure of as-prepared product was stable during processes of synthesis,exfoliation,self-assembly,and subsequent electrocatalytic OER.Rigorous electrochemical test proving the contributing catalytic active sites was located at the interface between Pt_(2)FeNi and DS^(-)-NiFe LDH,and the Ni and Fe were the major active elements while O atoms are adsorption sites.The formation of Pt_(2)FeNi nanoparticles could greatly prompt the reduction of Tafel slope.The best-performing Pt_(2)FeNi/DS^(-)-NiFe LDH with a Pt content of 0.98 wt%achieved low overpotential of 204 mV at 10 mA cm^(-2)and 262 mV at 50 mA cm^(-2).This work provides a convenient and effective strategy to create additional active sites for enhancing OER performance of NiFe LDH and make contribution to its wide application.

关键词： electrocatalysis NiFe Layered double hydroxides oxygen evolution reaction Pt_(2)FeNi nanoparticles

3D multicore-shell CoSn nanoboxes encapsulated in porous carbon as anode for lithium-ion batteries

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Chinese Chemical Letters 2022年第8期33卷 3925-3930页

作者： Daxu Zhang Gen Chen Haoji Wang Long Chen Ziwei Guo Zuxin Wen Ning Zhang xiaohe liu Renzhi Ma School of Materials Science and Engineering Central South UniversityChangsha 410083China School of Chemical Engineering and Energy Zhengzhou UniversityZhengzhou 450001China International Center for Materials Nanoarchitectonics(WPI-MANA) National Institute for Materials Science(NIMS)Ibaraki 305-0044Japan Key Laboratory of Electronic Packaging and Advanced Functional Materials of Hunan Province Central South UniversityChangsha 410083China

Due to its high theoretical capacity and appropriate potential platform,tin-based alloy materials are expected to be a competitive candidate for the next-generation high performance anodes of lithium-ion batteries.Nevertheless,the immense volume change during the lithium-ion insert process leads to severe disadvantages of structural damage and capacity fade,which limits its practical application.In this work,a three-dimensional(3 D)multicore-shell hollow nanobox encapsulated by carbon layer is obtained via a three-step method of hydrothermal reaction,annealing and alkali etching.During the electrochemical reactions,the CoSn@void@C nanoboxes provide internal space to compensate the volumetric change upon the lithiation of Sn,while the inactive component of Co acts as chemical buffers to withstand the anisotropic expansion of nanoparticles.Owing to the above-mentioned advantages,the elaborated anode delivers an excellent capacity of 788.2 m Ah/g at 100 m A/g after 100 cycles and considerable capacity retention of 519.2 mAh/g even at a high current density of 1 A/g after 300 cycles.The superior stability and high performance indicate its capability as promising anodes for lithium-ion batteries.

关键词： Lithium-ion battery CoSn nanoalloys Multicore-shell nanobox Hydrothermal reaction Sacrificial template