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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 fuels.Alkaline water electrolysis utilizing renewable energy sources has emerged as a means to obtain high-purity hydrogen.Nevertheless,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 contamination.Therefore,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 foam.The synthesized material exhibited remarkable performance,requiring a mere 476 mV to drive electrochemical water splitting at 100 mA cm^(-2)current density in alkaline solution.Furthermore,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

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Dimensional reduction enhances photocatalytic carbon dioxide reduction performance of metal-organic frameworks

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Nano Research 2024年第5期17卷 3653-3659页

作者： Kaiyue Ma Jixin Li Jinlu Liu Chunguang Li Zhan Shi Shouhua Feng State Key laboratory of inorganic synthesis and Preparative Chemistry College of ChemistryJilin UniversityChangchun 130012China

Metal-organic frameworks(MOFs)have shown significant potential as photocatalysts.It has been widely assumed that all catalytic active sites within MOFs are functional in photocatalytic reactions but for a three-dimensional MOF,whether the internal catalytic active sites can effectively absorb light and actively contribute to photocatalytic reactions remains to be explored.In this context,we synthesized a two-dimensional nanosheet MOF(2D-MOF)and a three-dimensional bulk MOF(3D-MOF)composed of Zr^(6) clusters and tetracarboxylic porphyrin(TCPP)by the approach described in the literature.Re(bpy)(CO)^(3)Cl(bpy=2,2’-bipyridine),which has remarkable CO_(2) photoreduction ability,was introduced to the two MOFs to create two new photocatalysts 2D-MOF-Re and 3D-MOF-Re,respectively.Photocatalytic CO_(2) reduction experiments show that based on the equal number of catalytic active sites,the CO turnover number(TON)of 2D-MOF-Re reaches 27.8 in 6 h,which is 50 times that of 3D-MOF-Re.The result shows that certain catalytic active sites inside the bulk MOF are inactive due to the inability to absorb light.This study illuminates the potential of the dimensional reduction approach in the design of photocatalysts to exploit the capabilities fully.

关键词： photocatalysis CO_(2)reduction metal-organic frameworks(MOFs) nanosheets light absorption

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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 storage.Seed-assisted synthesis is a very effective approach in promoting the crystallization of zeolites.In some cases,the target zeolite cannot be formed in the absence of seed zeolite.In 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 synthesis.In 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 syntheses.Finally,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

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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 synthesized.JLU-MOF130 features a three-dimensional(3D)architecture with a neb topology.JLU-MOF131 is characterized by a two-dimensional(2D)structure with an sql topology.JLU-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)NDC.The 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,respectively.The corresponding limit of detection(LOD)values are 1.17,1.36,and 14.59µmol/L.The 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,respectively.interestingly,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)

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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 future.Here,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 simultaneously.By reasonably controlling the cathode potential,the undesired water splitting reaction and furfural reduction side reactions are avoided.Under 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

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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) perovskite.It 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 activity.Such 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

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Total synthesis of a putative yuzurimine-type Daphniphyllum alkaloid C_(14)–epi-deoxycalyciphylline H

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Chinese Chemical Letters 2024年第4期35卷 336-339页

作者： Jingping Hu Jing Xu Shenzhen Grubbs Institute and Department of Chemistry and Guangdong Provincial Key laboratory of catalysis and Shenzhen Key laboratory of Small Molecule Drug Discovery and synthesis Southern University of Science and TechnologyShenzhen 518055China

One of the largest subfamilies within the famous Daphniphyllum alkaloid family is made up of the yuzurimine-type(or macrodaphniphyllamine-type) alkaloids. Their complex aza-polycyclic caged structures, several contiguous stereogenic centers, and vicinal all-carbon quaternary centers make these alkaloids formidable challenge for synthetic chemists. Recently, synthesis of these alkaloids has received extensive attention from our community. Herein, we wish to report the total synthesis of C_(14)–epideoxycalyciphylline H, a putative member of yuzurimine-type alkaloid subfamily. Key transformations employed in our approach include an intramolecular Prins reaction and a Pd-catalyzed enyne cycloisomerization. In addition, synthesis of a daphnezomine L-type alkaloid, paxdaphnidine A, was also studied.

关键词： Total synthesis Daphniphyllum alkaloids Yuzurimine-type alkaloids Prins reaction Enyne cycloisomerization

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Synergistic Co-doping effect of CNTs and PVP in Na_(4)MnCr(PO_(4))3 cathode as a strategy for improving the electrochemical performance of SIBs

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Chinese Chemical Letters 2024年第2期35卷 539-543页

作者： Ruoyu Chen Denys S.Butenko Shilin Li Xinyu Zhang Guangshe Li Igor V.Zatovsky Wei Han College of Physics State Key Laboratory of Inorganic Synthesis and Preparative ChemistryInternational Center of Future ScienceJilin UniversityChangchun 130012China Academy for Advanced Interdisciplinary Studies Southern University of Science and TechnologyShenzhen 518055China State Key laboratory of inorganic synthesis and Preparative Chemistry College of ChemistryJilin UniversityChangchun 130012China F.D.Ovcharenko Institute of Biocolloidal Chemistry NAS UkraineKyiv 03142Ukraine

In order to solve the contradiction between the rapidly growing energy demand and the excessive exploitation of fossil fuels,it is urgent to research and develops more environmentally friendly and efficient energy storage technologies.Therefore,the development of high-performance cathode materials to enhance the energy density of SIB is currently one of the most important topics of scientific research.Advanced high-voltage and low-cost cathode material for SIBs,a composite of carbon-coated Na_(4)MnCr(PO_(4))_(3)(NASICON-type),polyvinylpyrrolidone(PVP),and modified carbon nanotubes(CNTs)is prepared by sol-gel and freeze-drying method.Due to the high conductivity of CNTs,the conductivity of the composite is significantly improved,and its initial capacity is increased to 114 mAh/g at 0.5 C and 96 mAh/g at 5 C(Mn^(2+)/Mn^(4+)conversion for voltage windows 1.4-4.3 V).Moreover,the multi-electrons transfer of Cr^(3+)/Cr^(4+) and Mn^(2+)/Mn^(4+) can provide a high capacity of 165 mAh/g at 0.1 C and 102 mAh/g at 5 C in the high voltage window of 1.4-4.6 V.Furthermore,PVP can effectively inhibit the Jahn-Teller effect caused by Mn ion,making the composite have more excellent high-rate performance and stability.In addition,GITT,EIS and CV curves were drawn to better reveal the excellent kinetic properties of Na_(4)MnCr(PO_(4))_(3)@C@PVP@CNT cathode,and the mechanism of its performance improvement is deeply studied and discussed.Accordingly,the co-doping of CNTs and PVP is a simple way to high conductivity and fast charging of cathode materials for SIBs.

关键词： Sodium-ion batteries Na_(4)MnCr(PO_(4))_(3) Carbon nanotubes Polyvinylpyrrolidone Synergistic effect

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Integrating Zeolite and Layered Double Hydroxide for Highly Selective Catalytic Production ofγ-Valerolactone

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CCS Chemistry 2024年第3期6卷 652-662页

作者： Mingkun Gao Guoju Yang Guangyuan He Risheng Bai Jialiang Li Yinghao Liu Qiang Zhang Guangrui Chen Donghai Mei Jihong Yu State Key laboratory of inorganic synthesis and Preparative Chemistry College of ChemistryInternational Center of Future ScienceJilin UniversityChangchun 130012 School of Materials Science and Engineering Tiangong UniversityTianjin 300387

The production ofγ-valerolactone(GVL)from biomass derivatives levulinic acid(LA)based on acidbase metallic catalysts offers a sustainable pathway to the synthesis of valuable chemicals and biofuels.However,the development of efficient metallic catalysts with tunable Lewis acid–base and Brønsted acid sites remains a challenge.Herein,for the first time,we integrated zeolite and layered double hydroxide(LDH),in a core–shell structure,wherein zeolite and CoFe-LDH provided the Brønsted acidic sites and Lewis acid sites,respectively.Meanwhile,oxygen vacancies(OV_(x))acting as Lewis bases were generated on the surface of LDH via Ga doping.An efficient cascade catalytic reaction from LA to GVL was successfully achieved over the designed Beta@LDH-OVx catalyst,affording a superior conversion of LA(>99.9%)and an impressive selectivity to GVL(89.18%).Importantly,the“memory effect”of LDH endowed the catalyst with excellent regeneration of metal active sites.Density functional theory calculations revealed that the introduced OVx facilitated the adsorption of carbonyl oxygen in LA and boosted the production of GVL through the synergistic effect of acid/base sites in the composite catalyst.This work presents a rational design route for the construction of multifunctional catalysts by coupling zeolites and LDHs for highly selective catalytic conversion of biomass.

关键词： zeolite layered double hydroxide oxygen vacancies biomass γ-valerolactone

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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 area.Currently,the synthesis of PAF-1 is catalyzed by the Ni(COD)2/COD/bpy system,suffering from great instability and high cost.Herein,we developed an in situ reduction of the Ni(II)catalytic system to synthesize PAF-1 in low cost and high yield.The 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 detail.The efficiency and universality of this innovative catalyst system have also been demonstrated in other PAFs'synthesis.This 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

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