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Electrochemical synthesis of trimetallic nickel-iron-copper nanoparticles via potential-cycling for high current density anion exchange membrane water-splitting applications

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Journal of Energy chemistry 2024年第2期89卷 535-542,I0012页

作者： Ziqi Zhang Sheng Wan Hanbo Wang Jinghan He Ruige Zhang Yuhang Qi Haiyan Lu state key laboratory of inorganic synthesis and preparative chemistry College of ChemistryJilin UniversityChangchun 130012JilinChina

Hydrogen is known for its elevated energy density and environmental compatibility and is a promising alternative to fossil *** water electrolysis utilizing renewable energy sources has emerged as a means to obtain high-purity ***,electrocatalysts used in the process are fabricated using conventional wet chemical synthesis methods,such as sol-gel,hydrothermal,or surfactantassisted approaches,which often necessitate intricate pretreatment procedures and are vulnerable to post-treatment ***,this study introduces a streamlined and environmentally conscious one-step potential-cycling approach to generate a highly efficient trimetallic nickel-iron-copper electrocatalyst in situ on nickel *** synthesized material exhibited remarkable performance,requiring a mere 476 mV to drive electrochemical water splitting at 100 mA cm^(-2)current density in alkaline ***,this material was integrated into an anion exchange membrane watersplitting device and achieved an exceptionally high current density of 1 A cm^(-2)at a low cell voltage of2.13 V,outperforming the noble-metal benchmark(2.51 V).Additionally,ex situ characterizations were employed to detect transformations in the active sites during the catalytic process,revealing the structural transformations and providing inspiration for further design of electrocatalysts.

关键词： Electrocatalytic water splitting Hydrogen evolution reaction Oxygen evolution reaction Electrochemical synthesis Anion exchange membrane

The structure-directing role of heterologous seeds in the synthesis of zeolite

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Green Energy & Environment 2024年第5期9卷 792-801页

作者： Haoyang Zhang Binyu Wang Wenfu Yan state key laboratory of inorganic synthesis&preparative chemistry College of ChemistryJilin UniversityChangchun130012China

Zeolites have been widely used as catalysts,ion-exchangers,and adsorbents in chemical industries,detergent industry,steel industry,glass industry,ceramic industry,medical and healthﬁeld,and environmentalﬁeld,and recently applied in energy ***-assisted synthesis is a very effective approach in promoting the crystallization of *** some cases,the target zeolite cannot be formed in the absence of seed *** homologous seed-assisted synthesis,the structure of the seed zeolite is the same to that of the target zeolite,while the structure of the seed zeolite is different to that of the target zeolite in the heterologous seed-assisted *** this review,we brieﬂy summarized the heterologous seed-assisted syntheses of zeolites and analyzed the structure-directing effect of heterologous seeds and surveyed the“common composite building units(CBUs)hypothesis”and the“common secondary building units(SBUs)hypothesis”.However,both hypotheses cannot explain all observations on the heterologous seed-assisted ***,we proposed that the formation of the target zeolite does need nuclei with the structure of target zeolite and the formation of the nuclei of the target zeolite can be promoted by either the undissolved seed crystals with the same CBUs or SBUs to the target zeolite or by the facilitated appropriate distribution of the speciﬁc building units due to the presence of the heterologous seed that does not have any common CBUs and SBUs with the target zeolite.

关键词： Zeolite Heterologous seed synthesis Structure-directing effect

Regulation of Tumor Microenvironment Under Malignant Conditions:Application of nMOFs in Sonodynamic Therapy

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Chemical Research in Chinese Universities 2024年第4期40卷 611-626页

作者： YANG Yilin YAN Fei SHI Zhan state key laboratory of inorganic synthesis and preparative chemistry College of ChemistryJilin UniversityChangchun130012P.R.China

In this review,we delve into the intricate regulation of the tumor microenvironment(TME)under malignant conditions and explore the transformative potential of nanoscale metal-organic frameworks(nMOFs)in the realm of sonodynamic therapy(SDT).The TME serves as a dynamic milieu influencing tumor progression and therapeutic response,presenting formidable challenges,such as hypoxia,acidity,excess hydrogen peroxide,high expression of glutathione,and *** the exceptional attributes of nMOFs,including their tunable structures and biocompatibility,holds immense promise for enhancing SDT efficacy and reshaping the TME *** integrating nMOFs with SDT,researchers aim to assemble multiple functionalities in a single platform that enhance tumor cell eradication while counteracting unfavorable TME conditions and immune *** potential of nMOFs to revolutionize tumor therapies by precisely targeting TME and overcoming therapeutic barriers is underscored by an in-depth analysis of recent breakthroughs in the use of nMOFs-based sonosensitizers to remodulate TME to amplify the efficacy of SDT.

关键词： Sonodynamic therapy Metal-organic framework Tumor microenvironment Modification of sonosensitizer

Two Indium(III)-based Fluorescent Metal-Organic Frameworks for Highly Sensing Fe^(3+),2,4-DNP,and TNP

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Chemical Research in Chinese Universities 2024年第1期40卷 119-126页

作者： WANG Dan LI Wen LI Guanghua HUA Jia LIU Yunling state key laboratory of inorganic synthesis&preparative chemistry Jilin UniversityChangchun130012P.R.China

Two novel metal-organic frameworks(MOFs),JLU-MOF130([In(NH2−BDC)(Imi)(1H−Imi)]·DMF·H2O,NH2−H2BDC=2-aminobenzene-1,4-dicarboxylic acid,1H−Imi=1H-imidazole,DMF=N,N-dimethylformamide)and JLU-MOF131([In(1,4-NDC)(Imi)(1H−Imi)]·DMF0.5,1,4-H_(2)NDC=1,4-naphthalene-dicarboxylic acid),were ***-MOF130 features a three-dimensional(3D)architecture with a neb ***-MOF131 is characterized by a two-dimensional(2D)structure with an sql ***-MOF130 has excellent fluorescence detection performance towards Fe^(3+),2,4-dinitrophenol(2,4-DNP),and 2,4,6-trinitrophenol(TNP),but the fluorescence detection performance of JLU-MOF131 is further improved by converting NH2−H2BDC to more conjugated 1,4-H_(2)*** Stern-Volmer(SV)quenching constant(KSV)values of JLU-MOF130 sensing 2,4-DNP,TNP,and Fe^(3+)are 5.24×10^(4),4.44×10^(4),and 4.73×10^(3) L/mol,*** corresponding limit of detection(LOD)values are 1.17,1.36,and 14.59µmol/*** KSV values for JLU-MOF131 are 1.26×10^(5),9.02×10^(4),and 8.48×103 L/mol,and the corresponding LOD values are 0.35,0.42,and 3.60µmol/L,***,the emission wavelengths of the two MOFs obviously shift as the fluorescence emission intensities decrease upon the addition of 2,4-DNP and TNP,which can be applied in selective detection.

关键词： Metal-organic framework Fluorescence quenching Fe^(3+) 2 4-Dinitrophenol(2 4-DNP) 2 4 6-Trinitrophenol(TNP)

Linear paired electrolysis of furfural to furoic acid at both anode and cathode in a multiple redox mediated system

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Green Energy & Environment 2024年第1期9卷 104-113页

作者： Xinxin Li Linchuan Cong Haibo Lin Fangbing Liu Xiangxue Fu Hai-Chao Xu Nan Lin state key laboratory of inorganic synthesis and preparative chemistry Jilin UniversityChangchun 130012JilinChina state key laboratory of Physical chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005FujianChina

Implementing a new energy-saving electrochemical synthesis system with high commercial value is a strategy of the sustainable development for upgrading the bulk chemicals preparation technology in the ***,we report a multiple redox-mediated linear paired electrolysis system,combining the hydrogen peroxide mediated cathode process with the I2 mediated anode process,and realize the conversion of furfural to furoic acid in both side of the dividedﬂow cell *** reasonably controlling the cathode potential,the undesired water splitting reaction and furfural reduction side reactions are *** the galvanostatic electrolysis,the two-mediated electrode processes have good compatibility,which reduce the energy consumption by about 22%while improving the electronic efﬁciency by about 125%.This system provides a green electrochemical synthesis route with commercial prospects.

关键词： Multiple redox mediated system Linear paired electrolysis Furfural Furoic acid

Mechanism investigation of A-site doping on modulating electronic band structure and photocatalytic performance towards CO_(2) reduction of LaFeO_(3) perovskite

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Nano Research 2024年第5期17卷 3733-3744页

作者： Chi Cao Jinshuo Li Yang Hu Lin Zhang Wensheng Yang state key laboratory of inorganic synthesis and preparative chemistry College of ChemistryJilin UniversityChangchun 130012China Engineering Research Center for Nanomaterials Henan UniversityKaifeng 475004China

Three kinds of metal atoms with different valence electronic configurations,Bi(6s^(2)6p^(3)),Y(4d^(1)5s^(2)),and Ce(4f^(1)5d^(1)6s^(2)),were selected to investigate the effect of A-site(La^(3+))doping on electronic band structure,photoelectric properties,and photocatalytic performance of LaFeO_(3) *** was identified that the Bi doped LaFeO_(3) presented significantly improved photocatalytic activity towards the reduction of CO_(2),while the Y or Ce doped LaFeO_(3) displayed decreased photocatalytic activity compared to the pristine LaFeO_(3).It was revealed that doping of all the three metal atoms resulted in narrowed band gap and thus extended light absorption of LaFeO_(3) by lowering its conduction band minimum(CBM).The recombination rate and mobility of the charge carriers were represented by the relative effective mass(D)between holes and electrons for pristine and A-site doped LaFeO_(3).The doping of Bi resulted in increased D value,attributed to the Bi 6s electron states at the valence band maximum(VBM),and thus promoted separation and transfer of the charge carriers and improved photocatalytic activity of LaFeO_(3).In contrast,the doping of Ce resulted in significantly decreased D value,induced by the highly localized Ce 4f hole states at the CBM,and thus higher recombination rate of the charge carriers and decreased photocatalytic activity of LaFeO_(3).Furthermore,the Y doped LaFeO_(3) with a slightly decreased D value presented slightly increased recombination rate of the charge carriers and thus decreased photocatalytic *** a work provides new insights into the A-site doping in LaFeO_(3) perovskite,which should be helpful for optimizing the electronic band structure and activity of perovskite-type photocatalysts at atomic level.

关键词： A-site doping electronic band structure charge carrier behavior photocatalytic CO_(2)reduction perovskite-type photocatalytsts

Single-atom Zn confined in hierarchical hollow microstructure as an acid/base-resistant microwave absorption materials

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Nano Research 2024年第8期17卷 6785-6794页

作者： Yue Lou Jiao Li Xiaokun Li Zhenyu Zhu Zhan Shi Biao Xu School of chemistry and Chemical Engineering Nanjing University of Science and TechnologyNanjing 210094China state key laboratory of inorganic synthesis and preparative chemistry College of ChemistryJilin UniversityChangchun 130012China

Developing acid/base-resistant and low-price microwave-absorbing materials with lighter weight is highly desired for practical applications in extreme ***,we demonstrate the successful synthesis of the N-doped porous carbon(NC)material with hierarchical pore structure by the spray pyrolysis *** large specific surface area(SBET=707.53 m^(2)·g^(−1))of materials enables multiple scattering of incident electromagnetic waves,and N doping greatly enhances the electrical conductivity of the ***,single-atom Zn can adjust the local electronic structure of adjacent sites such as carbon and nitrogen atoms,induce the center of polarization,and thus change the dielectric and electronic properties of the host *** porous carbon coating of single-atom Zn avoids the deterioration of electromagnetic parameters caused by the accumulation of magnetic particles under high-temperature *** the same time,they can also be used in various complex environments,such as acidic and basic ***,NC-1000,with high surface area,low density,and good chemical stability,obtained a minimum reflection loss(RLmin)of−50.5 dB and an effective absorption bandwidth(EAB)exceeding 5.1 GHz at the thickness of 1.9 *** soaking in the strong acid and base solution,the electromagnetic wave absorption performance of the material decreased by<15%.Widely available raw materials and a simple preparation scheme are expected to expedite industrial mass production for this novel type of materials.

关键词： hierarchical hollow microstructure microwave absorption metal-organic framework(MOF) impedance matching singleatom Zn acid/base-resistant

Rational design of new in situ reduction of Ni(II)catalytic system for low-cost and large-scale preparation of porous aromatic frameworks

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Carbon Energy 2024年第5期6卷 105-113页

作者： Shanshan Wang Yue Wu Wenxiang Zhang Hao Ren Guangshan Zhu Heping Ma School of Chemical Engineering and Technology Xi'an Jiaotong UniversityXi'anChina state key laboratory of inorganic synthesis and preparative chemistry College of ChemistryJilin UniversityChangchunChina College of chemistry Northeast Normal UniversityChangchunChina

Porous aromatic framework 1(PAF-1)is an extremely representative nanoporous organic framework owing to its high stability and exceptionally high surface ***,the synthesis of PAF-1 is catalyzed by the Ni(COD)2/COD/bpy system,suffering from great instability and high ***,we developed an in situ reduction of the Ni(II)catalytic system to synthesize PAF-1 in low cost and high *** active Ni(0)species produced from the NiCl_(2)/bpy/NaI/Mg catalyst system can effectively catalyze homocoupling of tetrakis(4-bromophenyl)methane at the room temperature to form PAF-1 with high Brunauer-Emmett-Teller(BET)-specific surface area up to 4948 m^(2) g^(−1)(Langmuir surface area,6785 m2 g−1).The possible halogen exchange and dehalogenation coupling mechanisms for this new catalytic process in PAF's synthesis are discussed in *** efficiency and universality of this innovative catalyst system have also been demonstrated in other PAFs'*** work provides a cheap,facile,and efficient method for scalable synthesis of PAFs and explores their application for high-pressure storage of Xe and Kr.

关键词： adsorption carbon material nickel catalysis porous aromatic framework porous organic polymer

Metal–Organic Framework-Derived Hollow Nanocubes as Stable Noble Metal-Free Electrocatalyst for Water Splitting at High Current Density

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CCS chemistry 2024年第5期6卷 1324-1337页

作者： Ziqi Zhang Zhe Zhang Xiaobo Chen Hanbo Wang Haiyan Lu Zhan Shi Shouhua Feng state key laboratory of inorganic synthesis and preparative chemistry College of ChemistryJilin UniversityChangchun 130012 School of Engineering RMIT UniversityMelbourneVictoria 3000

Alkaline water electrolysis is an environmentally friendly and promising approach to produce ***,high cost,low efficiency,and poor stability are roadblocks to commercialization of *** work aims to design and develop a highly efficient,durable,and cost-effective electrocatalyst toward water splitting through modifying metal–organic *** electrocatalytic performance and stability surpass those of noble metal benchmarks at high current density(1–10 A·cm^(−2)).Theoretical calculations and in situ Raman spectra reveal the electronic structure of the synthesized catalyst and the mechanism of the catalytic reaction process,which rationalizes that the high catalytic activity and stability at high current are attributed to the unique electronic structure of cobalt regulated by copper and the protection provided by carbon nanotubes formed in situ,*** addition,this paper proposes that the desorption ability of the catalyst toward the products(H_(2)and O_(2)),rather than the adsorption ability toward the reactants(H^(+)or OH^(−)),is more important to the sustainable and stable electrochemical water splitting progress at high current density,which is a kinetic rather than thermodynamic dominating *** findings provide alternative insights to design and employ high performance catalysts to fuel hydrogen production as a clean energy source to tackle the global energy crisis.

关键词： metal-organic frameworks non-noble metal catalyst hydrogen evolution reaction oxygen evolution reaction electrocatalytic water splitting