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Multifunctional cellular carbon foams derived from chitosan toward self-cleaning, thermal insulation, and highly efficient microwave absorption properties

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nano Research 2024年第3期17卷 927-938页

作者： Beibei Zhan Yanling Hao Xiaosi Qi Yunpeng Qu Junfei Ding Jing-liang Yang Xiu Gong Yanli Chen Qiong Peng Wei Zhong College of Physics Guizhou Province Key Laboratory for Photoelectrics Technology and ApplicationGuizhou UniversityGuiyang 550025China Minzu Normal University of Xingyi Xingyi 562400China National laboratory of Solid State Microstructures and Jiangsu provincial laboratory for nanoTechnology Nanjing UniversityNanjing 210093China

To adapt the practical demand,designing and constructing the multifunctional microwave absorbers(MAs)is the key future direction of research and development.However,effective integrating the multiple functions into a single material remains a huge challenge.Herein,cellular carbon foams(CCFs)with different porous structures were elaborately designed and fabricated in high efficiency through a facile continuous freeze-drying and carbonization processes using a sustainable biomass chitosan as the precursor.The obtained results revealed that the thermal treated temperature and g-C_(3)N_(4) amount played a great impact on the carbonization degrees,pore sizes,and morphologies of CCFs,which led to their tunable electromagnetic(EM)parameters,improved conduction loss,and polarization loss abilities.Owing to the special cellular structure,the designed CCFs samples simultaneously displayed the strong absorption capabilities,broad absorption bandwidths,and thin matching thicknesses.Meanwhile,the as-prepared CCFs exhibited the strong hydrophobicity and good thermal insulation,endowing its attractive functions of self-cleaning and thermal insulation.Therefore,our findings not only presented a facile approach to produce different porous structures of CCFs,but also provided an effective strategy to develop multifunctional high-performance MAs on basis of three-dimensional CCFs.

关键词： multifunctional microwave absorbers carbon foams cellular structure self-cleaning thermal insulation

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Minimum-Modified Debye-Hückel Theory for Size-Asymmetric Electrolyte Solutions with Moderate Concentrations

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化学物理学报(英文) 2023年第5期36卷 553-560,I0001,I0002页

作者： Tiejun Xiao Yun Zhou guizhou provincial key laboratory of computational nano-material science Guizhou Synergetic Innovation Center of Scientific Big Data for Advanced Manufacturing TechnologyGuizhou Education UniversityGuiyang 550018China

A minimum-modified Debye-Hückel(DH)theory for electrolytes with size asymmetry is ***-pared with the conventional DH theory,the minimum-modified DH theory only introduces an extra surface charge density to capture the electrostatic effect of the size asymmetry of the electrolytes and hence facilitates a boundary element method for electrostatic potential calculation.This theory can distinguish the electrostat-ic energies and excess chemical potentials of ions with the same sizes but opposite charges,and is applied to a binary primitive electrolyte solution with moderate electrostatic coupling.Compared with the hyper-netted chain theory,the validity of this modified DH theory demonstrates significant improvement over the conventional DH theory.

关键词： Electrolyte solution Size-asymmetry Debye-Hückel theory Electrostatic ener-gy Chemical potential

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Slow Phase Transition-Induced Scan Rate Dependence of Spin Crossover in a Two-Dimensional Supramolecular Fe(III)Complex

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CCS Chemistry 2023年第2期5卷 412-422页

作者： Zhao-Yang Li Ying-Ying Wu Yao Li Jin-Hua Wang Arshia Sulaiman Mohammad Khurram Javed Ya-Chao Zhang Wei Li Xian-He Bu School of materials science and Engineering Nankai UniversityTianjin 300350 guizhou provincial key laboratory of computational nano-material science Guizhou Education UniversityGuiyang 550018 College of Chemistry Nankai UniversityTianjin 300071

Spin crossover(SCO)is commonly accompanied by a synchronous phase transition.A few phase transitioncoupled SCO compounds have been reported,yet the synergy between SCO and phase transition on different time scales has not been explored.Herein,we report an[Fe(H-5-Cl-thsa-Et)(5-Cl-thsa-Et)]·H2O(1·H2O;H2-5-Cl-thsa-Et=5-chloro-salicylaldehyde ethylthiosemicarbazone)Fe(III)complex that displays a two-dimensional supramolecular structure and SCO behavior above room temperature.Its dehydrated form1 exhibits a two-step spin transition with aplateau in the temperature-dependent magnetization(M−T)curve at room temperature and a 51 K thermal hysteresis loop(Tc↑↓=299/248 K)at a rate of 5 K/min.The improved SCOperformance in 1 could be attributed to the stronger intralayer but weaker interlayer interactions,which is supported by single-crystal structural analysis and density functional theory calculations.Remarkably,complex 1 displays an unusual scan rate-dependent SCO behavior at rates of 0.5−30 K/min,in whichM−T curveplateaus appear at lower scan rates(<10 K/min)but vanish at faster scan rates(≥10 K/min).Scan rate-dependent differential scanning calorimetry,powder X-ray diffractometry,timedependent magnetic moment decays,and infrared spectroscopy consistently reveal that the slow structural relaxation is coupled with a slowcrystallographic phase transition,which is the mechanism for the unusual scan rate-dependent SCO.

关键词： supramolecular two-dimensional structures scan rate dependence spin crossover slow phase transition

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Halogen chlorine triggered oxygen vacancy-rich Ni(OH)_(2) with enhanced reaction kinetics for pseudocapacitive energy storage

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Journal of Energy Chemistry 2023年第7期82卷 296-306,I0007页

作者： Jiangyu Hao Lijin Yan Liang Luo Qiaohui Liu Youcun Bai Yuying Han Yang Zhou Xuefeng Zou Bin Xiang School of Chemistry and Chemical Engineering Chongqing UniversityChongqing 400044China Analytical and Testing Center Chongqing UniversityChongqing 400044China guizhou provincial key laboratory of computational nano-material science Guizhou Education UniversityGuiyang 550018GuizhouChina School of materials science and Engineering Institute of Materials Science and DeviceSuzhou University of Science and TechnologySuzhou 215009JiangsuChina

Two-dimensional (2D)Ni(OH)_(2) nanosheets can theoretically expose their active sites of 100%.Whereas,their intrinsic easy accumulation and low conductivity lead to weak and unsustainable reaction kinetics.Herein,we propose a novel halogen chlorine-triggered electrochemical etching strategy to controllably manage the reaction kinetics of 2D Ni(OH)_(2) nanosheets(EE/Cl-Ni(OH)_(2)).It is found that halogen chlorine doping can adjust the interlamellar spacing flexibly and promote the lattice oxygen activation to achieve controlled construction of superficial oxygen defects at the adjustable voltage.The optimal EE/Cl-Ni(OH)_(2) electrode exhibits a high rate capability and excellent specific capacity of 206.9 mA h g^(-1) at 1 A g^(-1) in a three-electrode system,which is more than twice as high as the pristine Ni(OH)_(2).Furthermore,EE/Cl-Ni(OH)_(2) cathode and FeOOH@rGO anode are employed for developing an aqueous Ni-Fe battery with an excellent energy density of 83 W h kg^(-1),a high power density of 17051 W kg^(-1),and robust durability over 20,000 cycles.This strategy exploits a fresh channel for the ingenious fabrication of highefficiency and stable nickel-based deficiency materials for energy storage.

关键词： Ni(OH)_(2) Electrochemical etching Lattice defects High energy density Ni-Fe battery

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Understanding the hydrogen evolution reaction activity of doped single-atom catalysts on two-dimensional GaPS_(4) by DFT and machine learning

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能源化学:英文版 2023年第6期81卷 93-100,I0004页

作者： Tianyun Liu Xin Zhao Xuefei Liu Wenjun Xiao Zijiang Luo Wentao Wang Yuefei Zhang Jin-Cheng Liu College of Physics and Electronic science Guizhou Normal UniversityGuiyang 550025GuizhouChina Center for Rare Earth and Inorganic Functional materials School of Materials Science and Engineering&National Institute for Advanced MaterialsNankai UniversityTianjin 300350China Haihe laboratory of Sustainable Chemical Transformations Tianjin 300192China College of Information Guizhou University of Finance and EconomicsGuiyang 550025GuizhouChina guizhou provincial key laboratory of computational nano-material science Guizhou Education UniversityGuiyang 550018GuizhouChina

As a zero-carbon fuel,hydrogen can be produced via electrochemical water splitting using clean electric energy by the hydrogen evolution reaction(HER)process.The ultimate goal of HER catalyst is to replace the expensive Pt metal benchmark with a cheap one with equivalent activities.In this work,we investigated the possibility of HER process on single-atom catalysts(SACs)doped on two-dimensional(2D)GaPS_(4)materials,which have a large intrinsic band gap that can be regulated by doping and tensile strain.Based on the machine learning regression analysis,we can expand the prediction of HER performance to more catalysts without expensive DFT calculation.The electron affinity and first ionization energy are the two most important descriptors related to the HER behavior.Furthermore,constrain molecular dynamics with solvation models and constant potentials were applied to understand the dynamics barrier of HER process of Pt SAC on GaPS_(4)materials.These findings not only provide important insights into the catalytic properties of single-atom catalysts on GaPS_(4)2D materials,but also provides theoretical guidance paradigm for exploration of new catalysts.

关键词： Two-dimensional GaPS_(4) Hydrogen evolution reaction Single-atom catalysis First-principles calculation Machine learning

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Magic hybrid structure as multifunctional electrocatalyst surpassing benchmark Pt/C enables practical hydrazine fuel cell integrated with energy-saving H_(2)production

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escience 2022年第4期2卷 416-427页

作者： Ziyun Li Wentao Wang Qizhu Qian Yin Zhu Yafei Feng Yangyang Zhang Huaikun Zhang Mingyu Cheng Genqiang Zhang Hefei National Research Center for Physical sciences at the Microscale CAS Key Laboratory of Materials for Energy ConversionDepartment of Materials Science and EngineeringUniversity of Science and Technology of ChinaHefeiAnhui230026China guizhou provincial key laboratory of computational nano-material science Guizhou Education UniversityGuiyangGuizhou550018China

A hybrid catalyst structure can provide abundant active sites and tailored electronic properties,but the major challenge lies in achieving delicate control over its composition and architecture to improve the catalytic activity toward different electrochemical reactions simultaneously.Herein,we present the rational design of a magic hybrid structure with low Pt loading(5.90 wt%),composed of CoPt_(3)and CoPt nanoparticles supported on N-doped carbon(CoPt_(3)/CoPt⊂PLNC).Importantly,it shows superior multifunctional catalytic activity in alkaline conditions,requiring a low overpotential of 341 and 20 mV to achieve 10 mA cm^(−2)for the hydrazine oxidation reaction(HzOR)/hydrogen evolution reaction(HER),respectively,and it delivers a half-wave potential of 0.847 V for the oxygen reduction reaction(ORR).Theoretical calculations reveal that the metal-carbon hybrid modulates kinetic behavior and induces electron redistribution,achieving the energetic requirements for multiple electrocatalysis.We demonstrate sustainable H_(2)production utilizing solely the CoPt_(3)/CoPt⊂PLNC catalyst,without external electric power input,suggesting its inspiring practical utility.

关键词： Electrocatalysis Hybrid structure Fuel cell Hydrazine oxidation H_(2)production

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In-situ cation-inserted MnO_(2) with selective accelerated intercalation of individual H^(+) or Zn^(2+) ions in aqueous zinc ion batteries

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Journal of Energy Chemistry 2023年第7期82卷 88-102,I0003页

作者： Lijin Yan Baibai Liu Jiangyu Hao Yuying Han Chong Zhu Fuliang Liu Xuefeng Zou Yang Zhou Bin Xiang College of Chemistry and Chemical Engineering Chongqing UniversityChongqing 401331China College of Optoelectronic Engineering Chongqing UniversityChongqing 400044China guizhou Meiling Power Co. Zunyi 563099GuizhouChina Nanjing University of Aeronautics and Astronautics Nanjing 210016JiangsuChina guizhou provincial key laboratory of computational nano-material science Guizhou Normal UniversityGuiyang 550018GuizhouChina Analytical and Testing Center of Chongqing University Chongqing UniversityChongqing 401331China

The recognized energy storage mechanism of neutral aqueous zinc-manganese batteries is the co-insertion/extrusion of H^(+) and Zn^(2+) ions.However,modulating the kinetics of a single H^(+) or Zn^(2+) ion is scarce,which can provide meaningful insights into the energy storage mechanism of Zn ion batteries.Herein,a distinctive doubly electric field in-situ induced cationic anchoring of two-dimensional layered MnO_(2) is successfully constructed to modulate the insertion/extrusion of a single H^(+) or Zn^(2+) ion.As a result,regulating the intercalation of different metal ions can precisely achieve the accelerated induction for the individual H^(+) or Zn^(2+) ions intercalation/deintercalation.Moreover,the introduction of metal ions stabilizes the lattice distortion and alleviates the irreparable structural collapse,leading to an increase in the H^(+)/Zn^(2+) storage sites,efficiently diminishing the stagnation of the ordered structure and creating the more open channels,which is conducive to facilitating the diffusion of ions.This work delivers some innovative insights into pre-embedding strategies,and also serves as a precious reference for the cathode development of advanced aqueous batteries.

关键词： In-situ inductions Manganese dioxide Insertion mechanisms Zinc-ion batteries

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Li adsorption on monolayer and bilayer MoS_2 as an ideal substrate for hydrogen storage

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Chinese Physics B 2018年第6期27卷 320-328页

作者：张诚唐少龙邓明森都有为 School of Physics and Electronic science Guizhou Normal University Department of Physics Nanjing University guizhou provincial key laboratory of computational nano-material science Guizhou Education University

Based on the first-principles plane wave calculations, we show that Li adsorbed on monolayer and bilayer MoS2 forming a uniform and stable coverage can serve as a high-capacity hydrogen storage medium, and Li-coated MoS2 can be recycled by operations at room temperature due to Li having strength binding, big separation and is stable against clustering. The full Li coverage MoS2 system（2 ＊ 2 hexagonal MoS2 supercell） can reach up to eight H2 molecules on every side, corresponding to the gravimetric density of hydrogen storage up to 4.8 wt% and 2.5 wt% in monolayer and bilayer MoS2, respectively. The adsorption energies of hydrogen molecules are in the range of 0.10 e V/H2–0.25 e V/H2,which are acceptable for reversible H2 adsorption/desorption near ambient temperature. In addition, compared with light metals decorated low dimension carbon-based materials, the sandwiched structure of MoS2 exhibits the greatly enhanced binding stability of Li atoms as well as slightly decreased Li-Li interaction and thus avoids the problem of metal clustering.It is interesting to note that the Li atom apart from the electrostatic interaction, acts as a bridge of hybridization between the S atoms of MoS2 and adsorbed H2 molecules. The encouraging results show that such light metals decorated with MoS2 have great potential in developing high performance hydrogen storage materials.

关键词： MoS2 Li anchoring hydrogen storage first-principles

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A universal design for triggering the precise micro-structure reconstruction through in-situ electro-regulating to boost the pseudocapacitance of MnO_(2)

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Journal of Energy Chemistry 2022年第11期31卷 184-197,I0006页

作者： Lijin Yan Jiangyu Hao Baibai Liu Xuefeng Zou Qibin Wu Jin Hou Jizhou Duan Shicheng Wei Yang Zhou Bin Xiang Baorong Hou College of Chemistry and Chemical Engineering Chongqing UniversityChongqing 401331China College of Optoelectronic Engineering Chongqing UniversityChongqing 400044China guizhou provincial key laboratory of computational nano-material science Guizhou Normal UniversityGuiyang 550018GuizhouChina College of Chemistry and Chemical Engineering Ocean University of ChinaQingdao 266100ShandongChina key laboratory of Marine Environmental Corrosion and Bio-fouling Institute of OceanologyChinese Academy of SciencesQingdao 266071ShandongChina National key laboratory for Remanufacturing Army Academy of Armored ForcesBeijing 100072China Analytical and Testing Center of Chongqing University Chongqing UniversityChongqing 401331China

Developing a precise controllable strategy for modulating the micro-morphology,atom coordination environment,and electronic structure of electrode materials is crucial for the performance in the field of energy storage,yet still a tremendous challenge.Herein,a facile and universal in-situ electrochemical self-optimization design,electro-regulating,is designed to controllably produce electrode materials with abundant defects.Through detailed characterization studies,the microstructure of MnO_(2) is reconstructed after electro-regulating,which exhibits a structure of small fragments with numerous holes due to the partial self-dissolution of acidic oxides under an alkaline operating environment.Furthermore,the electro-regulating strategy not only presents the formation steps of numerous holes but is also accompanies by a number of O vacancies generation process due to the activation of an external electric field.This study provides a new inspiration for reasonably designing advanced functional electrode materials for various electrochemical applications and beyond.

关键词： Electro-regulating Microstructure reconstructed MnO_(2) Corrosion resistance Supercapacitors

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Rational design of large anomalous Nernst effect in Dirac semimetals

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npj computational materials 2023年第1期9卷 258-264页

作者： Panshuo Wang Zongxiang Hu Xiaosong Wu Qihang Liu Shenzhen Institute for Quantum science and Engineering and Department of Physics Southern University of Science and Technology518055 ShenzhenChina State key laboratory for Artificial Microstructure and Mesoscopic Physics Frontiers Science Center for Nano-optoelectronicsand Collaborative Innovation Center of Quantum MatterPeking University100871 BeijingChina Guangdong provincial key laboratory of computational science and material Design Southern University of Science and Technology518055 ShenzhenChina Shenzhen key laboratory of Advanced Quantum Functional materials and Devices Southern University of Science and Technology518055 ShenzhenChina

Anomalous Nernst effect generates a transverse voltage perpendicular to the temperature gradient.It has several advantages compared with the longitudinal thermoelectricity for energy conversion,such as decoupling of electronic and thermal transports,higher flexibility,and simpler lateral structure.However,a design principle beyond specific materials systems for obtaining a large anomalous Nernst conductivity(ANC)is still absent.In this work,we theoretically demonstrate that a pair of Dirac nodes under a Zeeman field manifests an odd-distributed,double-peak anomalous Hall conductivity curve with respect to the chemical potential and a compensated carrier feature,leading to an enhanced ANC compared with that of a simple Weyl semimetal with two Weyl nodes.Based on first-principles calculations,we then provide two Dirac semimetal candidates,i.e.,Na3Bi and NaTeAu,and show that under a Zeeman field,they exhibit a sizable ANC value of 0.4 Am^(-1)K^(-1) and 1.3 Am^(-1)K^(-1),respectively,near the Fermi level.Such an approach is also applicable to ferromagnetic materials with intrinsic Zeeman splitting,as exemplified by a hypothetical alloy NaFeTe2Au2,exhibiting an ANC as high as 3.7 Am^(-1)K^(-1) at the Fermi level.Our work provides a design principle with a prototype band structure for enhanced ANC pinning at the Fermi level,shedding light on the inverse design of other specific functional materials based on electronic structure.

关键词： structure Nernst Dirac

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