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Defect spinel oxides for electrocatalytic reduction reactions

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Nano Research 2024年第5期17卷 3547-3570页

作者： Zhijuan Liu Jinyu Guo Lu-yu Liu Fen Wang Zhijie Kong Yanyong Wang Henan key laboratory of Crystalline molecular Functional Materials Henan International Joint Laboratory of Tumor Theranostical Cluster MaterialsKey Laboratory of Special Environmental Functional Materials(Zhengzhou University)Ministry of EducationGreen Catalysis Centerand College of ChemistryZhengzhou UniversityZhengzhou 450001China State key laboratory of Chem/Bio-sensing and Chemometrics College of Chemistry and Chemical EngineeringHunan UniversityChangsha 410082China

Electrocatalytic reduction reactions play a crucial role in electrochemical energy conversion and storage technology,which are emerging technologies to ameliorate environmental *** oxides are widely explored in electrocatalytic oxidation reactions but have a poor intrinsic ability to reduction reactions,making their electrocatalytic ability less *** improve this,defect engineering is a valuable method for regulating the electronic structure and coordination ***,this manuscript discusses the use of defect spinel oxides in electrocatalytic reduction reactions,including the different types of defects,construction methods,and characterization *** also outlines the various applications of defect spinel oxides in different electrocatalytic reduction ***,it goes over the challenges and future outlooks for defect *** review aims to thoroughly explain how defect spinels work in electrocatalytic reduction reactions and serve as a helpful guide for creating effective electrocatalysts.

关键词： defect spinel oxides electrochemical reduction reactions electrocatalytic mechanism dynamic evolution

Developing silicon-based photocathodes for CO_(2) conversion

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Science China Chemistry 2024年第6期67卷 1904-1921页

作者： Weijie Zhuang Miao Kan Tao Meng Jinlong Zhang key laboratory for Advanced Materials and Joint International Research laboratory of Precision Chemistry and molecular engineering Feringa Nobel Prize Scientist Joint Research CenterSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai200237China Shanghai engineering Research Center for Multimedia Environmental Catalysis and Resource Utilization East China University of Science and TechnologyShanghai200237China

Photoelectrochemical(PEC)conversion of CO_(2) presents a promising avenue for solar-driven chemical fuel production,with silicon emerging as a cost-effective and high-light-absorbing material pivotal to this *** at exploring opportunities for industrializing PEC CO_(2) reduction(PEC-CO_(2)R)by minimizing reaction energy consumption,enhancing reaction efficiency and selectivity,this review summarizes recent advancements in developing Si-based photocathodes for PEC-CO_(2)*** outlines the fundamental principles,advantages,and limitations of Si photocathodes with key performance *** on this understanding,the strategies to enhance the performance of the PEC-CO_(2)R system,including light absorption,charge separation,and catalytic reactions are categorized as the interfacial modification,active site decoration,and protective layer *** design ideas of this advantageous three-layer structure in promoting the efficiency,stability,and selectivity have been ***,this review scrutinizes the influence of the photocathodic chemical *** review consolidates the mechanism insights and notable breakthroughs of various fuel generation processes within Si-based PEC-CO_(2)R *** this wealth of information offers an up-to-date perspective on the dynamic developments in silicon-based PEC-CO_(2) conversion and underscores the promising pathways toward the sustainable fuel synthesis from pollutant CO_(2).

关键词： photoelectrochemistry solar fuels silicon photocathodes carbon dioxide reduction microenvironment

Syntheses of new di-nuclear and tetra-nuclear lanthanide 9-anthracenecarboxylates:Magnetocaloric effect,slow magnetic relaxation and luminescent properties

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Journal of Rare Earths 2024年第6期42卷 1101-1109,I0004页

作者： Xing Liu Ruonan Yang Lu Zhang Jian Zhou Chunmei Huang Huahong Zou Zunhong Xiao Chongqing key laboratory of Inorganic Functional Materials College of ChemistryChongqing Normal UniversityChongqing401331China key laboratory for the Chemistry and molecular engineering of Medicinal Resources(Ministry of Education of China) School of Chemistry and Chemical Engineering of Guangxi Normal UniversityGuilin541004China School of Chemistry and Materials Guizhou Normal UniversityGuiyang550025China

Lanthanide complex-based materials with magnetic and luminescent properties have received a great deal of attention,owing to their importantly potential applications in diverse *** this work,the 9-anthracenecarboxylic acid(9-Haca)as bridging ligand was applied in combination with optically activeπ-conjugated 2,4,6-tri(2-pyridyl)-1,3,5-triazine(tptz)to construct a series of new di-nuclear and tetranuclear lanthanide 9-anthracenecarboxylates[La_(2)(9-aca)_(6)(tptz)_(2)(μ-H_(2)O)]·0.25H_(2)O(1),[Ln_(2)(9-aca)_(6)(tptz)_(2)(H_(2)O)_(2)]·0.5AQ·CH_(3)COOH_(2)H_(2)O[Ln=Sm(2a),Eu(2b),Gd(2c),Tb(2d),Dy(2e),Tm(2f);AQ=9,10-anthracenedione]and[Ln_(4)(9-aca)_(10)(tptz)_(2)(CH3COO)2]·H_(2)O[Ln=Eu(3a),Gd(3b),Dy(3c)].1 displays a di-nuclear centrosymmetric moiety[La_(2)(9-aca)_(6)(tptz)_(2)(μ-H_(2)O)]built up from two complex[La(9-aca)_(2)(tptz)]groups bridged by one H_(2)O molecule and two syn-syn-μ2-η1:η1-9-aca-bridging ligands,while 2a-2f are isostructural and co mprise another di-nuclear centrosymmetric moieties[Ln_(2)(9-aca)_(6)(tptz)_(2)(H_(2)O)_(2)]based on two complex[Ln(9-aca)_(2)(tptz)(H_(2)O)]groups connected by two syn-syn-μ2-η1:η1-9-aca-bridging ligands,3a-3c are isostructural and show tetra-nuclear centro symmetric moieties[Ln4(9-aca)10(tptz)2(CH3COO)2]containing three types of coordination modes of *** present compounds offer the only examples of lanthanide 9-anthracenecarboxylates decorated by optically active *** investigations of 2a,2c-2f,and 3b-3c indicate that 3c is typical of slow relaxation of the magnetization,while 2c and 3b show significant magnetocaloric effect(MCE)with the value of-ΔSm of 5.26 J/(kg·K)at 4 K and 15.65 J/(kg·K)at 2 K(ΔH=7 T),*** luminescent properties were also studied and reveal that the characteristic luminescent properties of the 7r-conjugated aromatic ligands are introduced into magnetic lanthanide 9-anthracenecarboxylates,simultaneously exhibiting slow magnetic relaxation(or MCE)and luminescen

关键词： Lanthanide complexes Luminescence Magnetic properties Magnetocaloric effect Slow magnetic relaxation Rare earths

Conversion of LiPSs Accelerated by Pt-Doped Biomass-Derived Hyphae Carbon Nanobelts as Self-Supporting Hosts for Long-Lifespan Li-S Batteries

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Energy & Environmental Materials 2024年第3期7卷 49-58页

作者： Fengfeng Han Liwen Fan Xinzhi Ma Huiqing Lu Lu Li Xitian Zhang Lili Wu key laboratory for Photonic and Electronic Bandgap Materials Ministry of EducationSchool of Physics and Electronic EngineeringHarbin Normal UniversityHarbin 150025China key laboratory of molecular Cytogenetics and Genetic Breeding of Heilongjiang Province School of Life Science and TechnologyHarbin Normal UniversityHarbin 150025China

Rechargeable Li-S batteries(LSBs)are emerging as an important alternative to lithium-ion batteries(LIBs),owing to their high energy densities and low cost;yet sluggish redox kinetics of LiPSs results in inferior cycle ***,we prepared multifunctional self-supporting hyphae carbon nanobelt(HCNB)as hosts by carbonization of hyphae balls of Rhizopus,which could increase the S loading of the cathode without sacrificing reaction *** platinum(Pt)nanoparticles were introduced into HCNBs(PtHCNBs)by ion-beam sputtering *** on the X-ray photoelectron spectroscopy analyses,the introduced trace Pt regulated the local electronic states of heteroatoms in *** kinetics investigation combined with operando Raman measurements revealed the accelerated reaction mechanics of sulfur *** from the synergistic catalytic effect and the unique structures,the as-prepared PtHCNB/MWNCT/S cathodes delivered a stable capacity retention of 77%for 400 cycles at 0.5 C with a sulfur loading of 4.6 mg cm^(-2).More importantly,remarkable cycling performance was achieved with an high areal S loading of 7.6 mg cm^(-2).This finding offers a new strategy to prolong the cycle life of LSBs.

关键词： high areal capacity high S loading hyphae carbon nanobelt lithium-sulfur battery operando Raman

Construction of multifunctional lanthanum manganese mixed nanoparticles mediated by ionic liquids for selective aerobic oxidation of cyclohexane

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Rare Metals 2024年第5期43卷 2205-2221页

作者： Hao Li Rui-Rui Zhang Ke-Xin Li Shuang Wei Yu-Mei Liu Rui-Xia Liu Beijing key laboratory of Ionic Liquids Clean Process CAS Key Laboratory of Green Process and EngineeringState Key Laboratory of Multiphase Complex SystemsInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China

Selective oxidation of alkanes to produce highvalue chemicals is an essential strategy and means to realize efficient utilization of *** this work,a strategy of lanthanum manganese mixed metal oxides(LMMO)regulated via a facile ionic liquid(IL)-assisted hydrothermal method was proposed to construct the multifunctional catalysts,which exhibited excellent catalytic performance in the selective aerobic oxidation of *** 8.9%cyclohexane conversion with 90%KA oi(cyclohexanol and cyclohexanone)selectivity was achieved over the optimal LMMO catalyst under mild *** effects of anion type,carbon chain length and concentration of ILs on the structure and properties of catalysts were investigated through various characterizations,indicating the structure-directing and template effect of ILs on the multifunctional *** formation of self-assembled spherical nanoparticles followed the"dissolution-nucleation-proliferation"mechanism with the introduction of 1-butyl-3-methylimidazolium hydrogen sulfate,ascribing the synergistic effect between the microenvironment of ILs and the hydrothermal ***,the high reactive oxygen concentration redox capacity,and suitable basic sites of LMMO catalysts mediated by ILs enhance the activation of C-H bonds and molecular oxygen,simultaneously influencing the adsorption and desorption of the substrate.A comprehensive understanding of the high KA oil selectivity and radical reaction mechanism was elucidated based on in situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS)and radical trapping *** recycling and regeneration experiments further illuminated that the removal of adsorbed cyclohexanone acting on the LMMO catalyst was the key to achieve high KA oil selectivity.

关键词： Ionic liquids Nanoparticle Multifunctional catalyst Cyclohexane oxidation

Suppression of current-induced membrane discharge of bipolar membranes by regulating ion crossover transport

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Journal of Energy Chemistry 2024年第9期96卷 387-395页

作者： Tingting Yu Haolan Tao Jingkun Li Cheng Lian Honglai Liu State key laboratory of Chemical engineering Shanghai Engineering Research Center of Hierarchical NanomaterialsSchool of Chemical EngineeringEast China University of Science and TechnologyShanghai 200237China School of Chemistry and molecular engineering East China University of Science and TechnologyShanghai 200237China

Bipolar membranes(BPMs)exhibit the unique capability to regulate the operating environment of electrochemical system through the water dissociation-combination ***,the industrial utilization of BPMs is limited by instability and serious energy *** current-induced membrane discharge(CIMD)at high-current conditions has a negative influence on the performance of anion-exchange membranes,but the underlying ion transport mechanisms in the BPMs remain ***,the CIMD-coupled Poisson-Nernst-Planck(PNP)equations are used to explore the ion transport mechanisms in the BPMs for both reverse bias and forward bias at neutral and acid-base *** is demonstrated that the CIMD effect in the reverse-bias mode can be suppressed by enhancing the diffusive transport of salt counter-ions(Na^(+)and Cl^(−))into the BPMs,and that in the forward-bias mode with acid-base electrolytes can be suppressed by matching the transport rate of water counter-ions(H_(3)O^(+)and OH^(−)).Suppressing the CIMD can promote the water dissociation in the reverse-bias mode,as well as overcome the plateau of limiting current density and reduce the interfacial blockage of salt co-ions(Cl^(−))in the anion-exchange layer in the forward-bias mode with acid-base *** work highlights the importance of regulating ion crossover transport on improving the performance of BPMs.

关键词： Bipolar membranes Current-induced membrane discharge Salt ion crossover Diffusion-migration-reaction process

Steric hindrance shielding viologen against alkali attack in realizing ultrastable aqueous flow batteries

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Journal of Energy Chemistry 2024年第10期97卷 529-534页

作者： Liwen Wang Kai Wan Xianzhi Yuan Zhipeng Xiang Zhiyong Fu Zhenxing Liang Guangdong Provincial key laboratory of Fuel Cell Technology School of Chemistry and Chemical Engineering South China University of Technology State key laboratory of Pulp and Paper engineering South China University of Technology Guangdong Provincial laboratory of Chemistry and Fine Chemical engineering Jieyang Center

Viologens known as a kind of promising negolyte materials for aqueous organic redox flow batteries,face a critical stability challenge due to the SN2 nucleophilic attack by hydroxide ions（OH-） during the battery *** this work,a N-cyclic quaternary ammonium-grafted viologen molecule,viz.1,1'-bis（4,4'-dime thylpiperidiniumyl）-4,4'-bipyridinium tetrachloride(（DBPPy）Cl4),is developed by the molecular engineering *** obtained（DBPPy）Cl4molecule shows a decent solubility of 1.84 M and a redox potential of-0.52 V ***/AgCl,Experimental and theoretical results reveal that the grafted N-cyclic quaternary ammonium groups act as the steric hindrance to prevent nucleophilic attack by OH-,increasing the alkali resistance of the electroactive *** symmetrical battery with 0.50 M（DBPPy）Cl4shows negligible decay during the 13-day cycling *** demonstration,the flow battery utilizing 1.0 M（DBPPy）Cl4as the negolyte and 1-（1-oxyl-2,2',6,6'-tetramethylpiperidin-4-yl）-1'-(3-（trimethylammonio）propyl)-4,4'-bipyridinium trichloride as the posolyte exhibits a high capacity retention rate of 99.99% per cycle at 60 mA cm-2.

关键词： Alkali resistance Aqueous organic flow batteries Stability Steric hindrance Viologen

Understanding the Interfacial Energy Structure and Electron Extraction Process in Inverted Organic Solar Cells with Phosphine-Doped Cathode Interlayers

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Chinese Journal of Chemistry 2024年第12期42卷 1347-1354页

作者： Yi Yang Jingwen Wang Yang Xiao Bowei Xu Jianhui Hou State key laboratory of Polymer Physics and Chemistry Beijing National Laboratory for Molecular SciencesInstitute of ChemistryChinese Academy of SciencesBeijing 100190China State key laboratory of Chemical Resource engineering College of Materials Science and EngineeringBeijing University of Chemical TechnologyBejing 100029China University of Chinese Academy of Sciences Beijing 100049China

Comprehensive Summary Cathode interlayers(CILs)play an essential role in achieving efficient organic solar cells(OSCs).However,the electronic structure at the electrode/CIL/active layer interfaces and the underlying mechanisms for electron collection remain unclear,which becomes a major obstacle to develop high-performance ***,we investigate the relationship of the electron collection abilities of four cross-linked and n-doped CILs(c-NDI:P0,c-NDI:P1,c-NDI:P2,c-NDI:P3)with their electronic structure of space charge region at heterojunction *** accurately calculating the depletion region width according to the barrier height,doping density and permittivity,we put forward that the optimal thickness of CIL should be consistent with the depletion region width to realize the minimum energy *** a result,the depletion region width is largely reduced from 13 nm to 0.8 nm at the indium tin oxide(ITO)/c-NDI:P0 interface,resulting in a decent PCE of 17.7%for the corresponding inverted OSCs.

关键词： Organic solar cells Cathode interlayer Depletion region width Electric conductivity Electron transport Electron transfer Electron extraction process

Readily prepared and processed multifunctional MXene nanocomposite hydrogels for smart electronics

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SmartMat 2024年第2期5卷 103-114页

作者： Jiahui Huang Xianwu Huang Peiyi Wu State key laboratory for Modification of Chemical Fibers and Polymer Materials College of Chemistry and Chemical EngineeringCenter for Advanced Low-Dimension MaterialsDonghua UniversityShanghaiChina State key laboratory of molecular engineering of Polymers Department of Macromolecular Science and Laboratory of Advanced MaterialsFudan UniversityShanghaiChina

Booming sophisticated robotics and prosthetics put forward high requirements on soft conductive materials that can bridge electronics and biology,those soft conductive materials should imitate the mechanical properties of biological tissues and build information transmission *** now,it remains a great challenge to handle the trade-off among ease of preparation,high conductivity,processability,mechanical adaptability,and external stimuli ***,a kind of readily prepared and processed multifunctional MXene nanocomposite hydrogel is reported,which is prepared via the fast gelation of cationic monomer initiated by delaminated MXene *** gelation time can be adjusted(several seconds to minutes)based on the MXene *** adjusting the MXene ratio,the resulting nanocomposites are ultrastretchable(>5000%),three-dimensional(3D)printable,and show outstanding mechanical and electrical *** expected,the integration of multifunctional systems onto various substrates(e.g.,gloves and masks)is further demonstrated via 3D printing and could achieve diverse sensory capabilities toward strain,pressure,and temperature,showing great prospects as smart flexible electronics.

关键词： 3D printable electronics MXene polymeric hydrogels stretchable and conductive