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Efficient and stable PtFe alloy catalyst for electrocatalytic methanol oxidation with high resistance to CO

Journal of Energy chemistry 2024年第3期90卷 327-336,I0008页

作者： Qian Yang Sifan Zhang Fengshun Wu Lihua Zhu Guang Li Mingzhi Chen An Pei Yingliang Feng Jiangxi Provincial Key Laboratory of Functional Molecular materials chemistry College of Chemistry and Chemical EngineeringFaculty of Materials Metallurgy and ChemistryJiangxi University of Science and TechnologyGanzhou 341000JiangxiChina college of chemistry and chemical engineering Xiamen UniversityXiamen 361005FujianChina

Direct methanol fuel cells(DMFC) are widely considered to be an ideal green energy conversion device but their widespread applications are limited by the high price of the Pt-based catalysts and the instability in terms of surface CO toxicity in long-term ***,the PtFe alloy nanoparticles(NPs) with small particle size(~4.12 nm) supported on carbon black catalysts with different Pt/Fe atomic ratios(Pt_(1)Fe_(2)/C,Pt_(3)Fe_(4)/C,Pt_(1)Fe_(1)/C,and Pt_(2)Fe_(1)/C) are successfully prepared for enhanced anti-CO poisoning during methanol oxidation reaction(MOR).The optimal atomic ratio of Pt/Fe for the MOR is 1:2,and the mass activity of Pt_(1)Fe_(2)/C(5.40 A mg_(Pt)^(-1)) is 13.5 times higher than that of conventional commercial Pt/C(Pt/C-JM)(0.40 A mg_(Pt)^(-1)).The introduction of Fe into the Pt lattice forms the PtFe alloy phase,and the electron density of Pt is reduced after forming the PtFe ***-situ Fourier transform infrared results indicate that the addition of oxyphilic metal Fe has reduced the adsorption of reactant molecules on Pt during the *** doping of Fe atoms helps to desorb toxic intermediates and regenerate Pt active sites,promoting the cleavage of C-O bonds with good selectivity of CO_(2)(58.1%).Moreover,the Pt_(1)Fe_(2)/C catalyst exhibits higher CO tolerance,methanol electrooxidation activity,and long-term stability than other Pt_(x)Fe_(y)/C catalysts.

关键词： Alloy catalyst PtFe Methanol oxidation In-situ FTIR CO resistance

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Polypyride intercalation boosting the kinetics and stability of V3O7·H2O cathodes for aqueous zinc-ion batteries

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Journal of Energy chemistry 2024年第10期97卷 361-370页

作者： Qingqing He Jie Bai Mengda Xue Yanxin Liao Huayu Wang Mujun Long Lingyun Chen Department of Applied chemistry School of Chemistry and Chemical Engineering Chongqing University Laboratory of materials and Metallurgy College of Materials Science and Engineering Chongqing University

V3O7·H2O（VO） is a high capacity cathode material in the field of aqueous zinc ion batteries（AZIBs）,but it is limited by slow ion migration and low electrical *** this paper,polypyridine（PPyd） intercalated VO with nanoribbon structure was prepared by a simple in-situ pre-intercalation,which is noted *** total density of states（TDOS） shows that after the pre-intercalation of PPyd,an intermediate energy level appears between the valence band and conduction band,which provides a step that can effectively reduce the band gap and enhance the electron ***,the density functional theory（DFT） results found that Zn2+is more easily de-intercalated from the V-O skeleton,which proves that the embeddedness of PPyd improves the diffusion kinetics of Zn2+.Electrochemical studies have shown that VO-PPyd cathode materials exhibit excellent rate performance(high specific capacity of 465 and 192 mA h g-1at 0.2 and 10 A g-1,respectively) and long-term cycling performance（92.7%capacity retention rate after 5300 cycles）,due to their advantages in structure and *** importantly,the energy density of VO-PPyd//Zn at 581 and 5806 W kg-1is 375 and 247 W h kg-1,***-PPyd exhibits excellent electrochemical properties compared to previously reported vanadium based cathodes,which makes it highly competitive in the field of high-performance cathode materials of AZIBs.

关键词： Aqueous zinc ion batteries DFT calculation Electrical conductivity Ion migration Polypyridine V3O7·H2O

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PVDF-assisted pyrolysis strategy for corrugated plate oxygen electrocatalysis nanoreactor:Simultaneously realizing efficient active sites and rapid mass transfer

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Journal of Energy chemistry 2024年第10期97卷 612-621页

作者： Chenxi Xu Liang Chen Haihui Zhou Shifeng Qin Zhaohui Hou Yangyang Chen Jiale Sun Junwei Xu Zhongyuan Huang college of chemistry and chemical engineering Hunan University college of materials Science and Technology Central South University of Forestry and Technology Key Laboratory of Hunan Province for Advanced Carbon-based Functional materials School of Chemistry and Chemical Engineering Hunan Institute of Science and Technology

Though Zn-air batteries(ZABs) are one of the most promising system for energy storage and conversion,challenge still persists in its commercial application due to the sluggish kinetics of oxygen reduction/evolution reaction(ORR/OER).Hereby,a polyvinylidene fluoride(PVDF)-assisted pyrolysis strategy is proposed to develop a novel corrugated plate-like bifunctional electrocatalyst using two-dimensional zeolitic imidazolate frameworks(2D ZIF-67) as the *** employed PVDF plays an important role in inheriting the original 2D structure of ZIF-67 and modulating the composition of the final *** a result,a corrugated plate-like electrocatalyst,high-density Co nanoparticles decorated 2D Co,N,and F tri-doped carbon nanosheets,can be *** acquired electrocatalyst enables efficient active sites and rapid mass transfer simultaneously,thus showing appreciable electrocatalytic performance for rechargeable Zn-air ***,our proposed strategy offers a new perspective to the design of advanced oxygen electrocatalysts.

关键词： Active sites Corrugated plate Mass transfer Oxygen electrocatalyst Zn-air batteries

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π-conjugated chromophore functionalized high-nuclearity titanium-oxo clusters containing structural unit of anatase for photocatalytic selective oxidation of sulfides

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Rare Metals 2024年第4期43卷 1736-1746页

作者： Ling-Rong Liao Dong-Chun Zheng Pin-Xi Ou Qi-Xin Zhao Wei-Min Xuan Qi Zheng State Key Laboratory for Modification of chemical Fibers and Polymer materials&college of materials Science and engineering Donghua UniversityShanghai201620China State Key Laboratory for Modification of chemical Fibers and Polymer materials and college of chemistry and chemical engineering Donghua UniversityShanghai 201620China

N-doping has significant influence in manipulating the properties of TiO_(2),and this has stimulated the development of N-donor-functionalized titanium-oxo clusters(TOCs)as molecular models to study the structure-property ***,the structural type and photoresponsive application are still limited for such TOCs,especially regarding the high-nuclearity TOCs that contain structure unit of TiO_(2)for ***,we showed the synthesis of a series of high-nuclearity TOCs 1-3 compounds usingπ-conjugated 1,10-phenanthroline(phen)as chromophore and N-donor functional *** 1 features cocrystal structure composed of one[Ti_(26)]~(2+)and half[Ti_(22)]~(2+),which renders it as the first cocrystallized TOC containing two positively charged species and phen-functionalized TOC showing the highest nuclearity up to 37 Ti *** adjusting the synthetic conditions,the individual{Ti_(22)}and{Ti_(26)}clusters can also be isolated as Compounds 2 and 3,*** core structure of{Ti_(22)}is mainly constructed from four lacunary{Ti_(4)}derived from pentagonal{Ti(Ti)_5}unit,while{Ti_(26)}is built from four complete{Ti(Ti)_5}***,a{Ti_8O_(14)}structure unit of anatase TiO_(2)can be identified in{Ti_(26)}.Based on the unique structural features and proper photophysical and photochemical properties of Compounds 1-3,they are applied for photocatalytic *** to the presence of anatase structure unit in{Ti_(26)}and the synergistic effect from{Ti_(22)}and{Ti_(26)},the catalytic performance presents in the order of Compound 1>Compound 3>Compound *** work provides excellent models to understand the structureproperty relationship from the perspective of cocrystallization and Ti-O binding model and will further promote the application of TOCs as functional catalysts for organic transformation.

关键词： Titanium-oxo cluster Molecular model of anatase TiO_(2) High nuclearity π-conjugated chromophore Photocatalytic sulfoxidation

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Molecular solid solution of lanthanide-titanium-oxo clusters with enhanced photocatalytic hydrogen evolution

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Science China chemistry 2024年第2期67卷 529-535页

作者： Rong Chen Chao-Long Chen Hui Zhang Zi-Han Wang Fu-Li Sun Ming-Hao Du Gui-Lin Zhuang Cheng Wang La-Sheng Long Lan-Sun Zheng Xiang-Jian Kong Collaborative Innovation Centre of chemistry for Energy materials State Key Laboratory of Physical chemistry of Solid Surfaces and Department of chemistry College of Chemistry and Chemical EngineeringXiamen UniversityXiamen361005China college of chemical engineering Zhejiang University of TechnologyHangzhou310032China

Molecular solid solutions of metal clusters containing different metal centers with well-defined structures can accurately regulate the HOMO-LUMO gap,but are rarely ***,a series of colorless lanthanide-titanium-oxo clusters Ln_(2)Ti_4(μ_(2)-O)_(2)(μ_(3)-O)_4(Piv)_(10)(THF)_(2)(Ln_(2)Ti_4,Ln = Eu,Gd,Tb,and Ce,HPiv = pivalic acid) were synthesized by the reaction of pivalic acid with Ln(Ac)_(3) and titanium *** light yellow crystal of cluster solid solutions Eu_(2)Ti_(4-x)Cd_(x),containing a mixture of Eu_(2)Ti_4 and Eu_(2)Ti_(3)Cd,was obtained by in situ doping Cd^(2+) and S^(2–).Eu_(2)Ti_(3.92)Cd_(0.08) displays efficient photocatalytic hydrogen evolution activity without a co-catalyst,which is up to 2.6 times that of Eu_(2)Ti_*** time-resolved transient absorption spectroscopy and spin-polarized density functional calculations showed that the enhanced photocatalytic performance of Eu_(2)Ti_(4-x)Cd_(x) can be attributed to the narrower HOMO-LUMO gap and lower LUMO position than that of Eu_(2)Ti_*** studyprovides an in situ doping method to realize the simple preparation of cluster solid solution.

关键词： molecular solid solution lanthanide-titanium-oxo clusters photocatalytic hydrogen evolution

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Two-dimensional C2N-based single-atom catalyst with complex microenvironment for enhanced electrochemical nitrogen reduction:A descriptor-based design

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Journal of Energy chemistry 2024年第10期97卷 110-119页

作者： Enduo Dai Wei An Ruixian Guo Xugen Shi Yunyi Li Yibo Wang Mingming Liu college of chemistry and chemical engineering Shanghai University of Engineering Science

The catalytic descriptor with operational feasibility is highly desired towards rational design of high-performance catalyst especially the electrode/electrolyte solution interface working under mild ***,we demonstrate that the descriptor Ω parameterized by readily accessible intrinsic properties of metal center and coordination is highly operational and efficient in rational design of single-atom catalyst（SAC） for driving electrochemical nitrogen reduction（NRR）.Using twodimensional metal（M）-BxPySzNm@C2N as prototype SAC models,we reveal that*N2+（H++e-）→*N2H acts predominantly as the potential-limiting step（PLS） of NRR on M-B2P2S2@C2N and M-B1P1S1N3@C2N regardless of the distinction in coordination *** the 28 screened M active sites,with Ω values close to the optimal 4,M-B2P2S2@C2N(M=V（Ω=3.53）,Mo（Ω=5.12）,and W（Ω=3.92）) and M-B1P1S1N3@C2N(M=V（Ω=3.00）,Mo（Ω=4.34）,and W（Ω=3.32）) yield the lowered limiting potential（UL） as-0.45,-0.54.-0.36,-0.58,-0.25,and-0.24 V,respectively,thus making them the promising NRR *** importantly,these SACs are located around the top of volcano-shape plot of ULversus Ω,re-validating Ω as an effective descriptor for accurately predicting the high-activity NRR SACs even with complex *** study unravels the relationship between active-site structure and NRR performance via the descriptor Ω,which can be applied to other important sustainable electrocatalytic reactions involving activation of small molecules via σ-donation and π*-backdonation mechanism.

关键词： Descriptor DFT Electrocatalysis N2 reduction Single-atom catalyst

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Tunable Phase Structure of Side-chain Liquid Crystalline Polymers Enabled by Molecular engineering of Dual Mesogenic Cores

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Chinese Journal of Polymer Science 2024年第10期42卷 1459-1469页

作者： Wen-Huan Yao Lan-Sheng Liu Jie Zhao Yan-Xia Wang An-Zhi Ma Zheng-Rui Ma Lan-Ying Zhang Ruo-Chen Lan college of chemistry and chemical engineering Hunan University Key Laboratory of Eco-Functional Polymer materials of the Ministry of Education Key Laboratory of Eco-Environmental Polymer Materials of Gansu ProvinceCollege of Chemistry and Chemical Engineering Northwest Normal University Department of materials Science and engineering College of Engineering Peking University Institute of Advanced materials & Key Lab of Fluorine and Silicon for Energy materials and chemistry of Ministry of Education College of Chemistry and Chemical Engineering Jiangxi Normal University

A series of novel side-chain liquid crystalline (SCLC) copolymers were synthesized by attaching two distinct mesogenic units, namely a chiral cholesteryl-based monomer (M1) and an achiral biphenyl-based monomer (M2), to a poly(3-mercaptopropylmethylsiloxane)(PMMS) backbone via thiol-ene click chemistry. The influence of side chain composition on the self-assembly behavior and phase structures of these SCLC copolymers was systematically investigated using different instrument. Results indicate that three distinct liquid crystalline phases and four unique molecular configurations were identified within the polymer series, with the emergence of the liquid crystalline phase being a synergistic outcome of the two distinct side chains. This study underscores the critical influence of side chain dimensions, rigidity, and spatial volume on the self-assembly structures and phase characteristics of liquid crystalline polymers, providing valuable insights for the rational design and development of advanced functional materials with tailored properties.

关键词： Chiral molar ratio Liquid crystalline copolymers Phase structure Self-assembly

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Highly sensitive fluorescent sensing and photocatalytic degradation performance of two-dimensional Tb-organic network

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Journal of Rare Earths 2024年第2期42卷 303-313,I0003页

作者： Ting Gao Zhihu Ma Yixia Ren Zhixiang Wang Meili Zhang Xiaoli Chen Jijiang Wang Laboratory of New Energy and New Function materials Shaanxi Key Laboratory of Chemical Reaction EngineeringCollege of Chemistry and Chemical EngineeringYan'an UniversityYan'an716000China

A novel tetra-nuclear Tb-organic network,named as [Tb_(4)(2-pyia)_(6)(HAc)_(0.5)(2,2'-bipy)(H_(2)O)_(4.5)]·2,2'-bipy·H_(2)O(1),was synthesized hydrothermally based on 5-(pyridin-2-ylmethoxy) isophthalic acid(H_(2)pyia) and 2,2'-bipyridine(2,2'-bipy) ligands,and characterized by single crystal X-ray diffraction,thermogravimetric(TG) analyses,powder X-ray diffraction(PXRD) and infrared(IR) technology.1 possesses a two-dimensional network based on the tetra-nuclear inorganic building units,and the π-πstacking interactions between the pyia^(2-) ligands and the guest 2,2'-bipy molecules play an important role in the forming of 3D supramolecular structure.1 exhibits excellent fluorescent sensing performance for Fe^(3+)(1.26×10^(-8) mol/L),Cr_(2)O_(7)^(2-)(8.1×10^(-7) mol/L),2,4,6-trinitrophenol(TNP)(2.71×10^(-8) mol/L)and tetracycline(TCT)(2.76×10^(-7) mol/L) in aqueous solution with lower detection *** sensing mechanisms of 1 were investigated by density functional theory(DFT) calculations,ultraviolet-visible(UV-Vis) diffuse reflectance spectroscopy,PXRD and fluorescent lifetime *** activated product of 1 was prepared by heating at 255℃ under constant pressure and used to photo-catalytically degrade *** 1 and the activated one have good photocatalytic degradation performance for TCT with degradation rates of 84.29% and 96.07%,*** photocatalytic mechanisms were discovered by UV-Vis diffuse reflectance spectroscopy and radical trap *** Tb-organic framework might be an excellent multifunctional fluorescent sensor and a good photocatalytic agent for TCT degradation in the future.

关键词： Tb-organic network Fluorescent sensing Photocatalytic degradation Rare earths

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Zeolite polymer membrane as protective interface for Mg battery

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Rare Metals 2024年第9期43卷 4636-4638页

作者： Hai-Xia Wu Kai-Lu Guo college of chemistry and chemical engineering Henan Key Laboratory of Function-Oriented Porous MaterialsLuoyang Normal University

Excessive electrolyte decomposition seriously determines the performance of high-voltage Mg batteries. In Nazar?s work, the strategy using a zeolite polymer membrane as a protective interface was proposed to restrain the electrolyte decomposition. This strategy could boost Mg plating/stripping performance up to 6000 h in zeolite/Mg|zeolite/Mg symmetric cells and 91%capacity retention in zeolite/Mg||Mo3S4battery after 200 *** storage devices have been intensively explored because of their important roles in our daily lives [1D3].

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FeNi Prussian blue analogues on highly graphitized carbon nanosheets as efficient glucose sensors

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Rare Metals 2024年第6期43卷 2730-2738页

作者： Jin-Hang Xue Qiu-Hong Sun Cheng Han Yuan-Dong Yang Shao-Jie Xu Qi-Peng Li Jin-Jie Qian college of Life and Environmental Science Wenzhou UniversityWenzhou 325000China college of chemistry and materials engineering Wenzhou UniversityWenzhou 325000China college of chemistry and chemical engineering Zhaotong UniversityZhaotong 657000China

Meeting the continuous glucose monitoring requirements of individuals necessitates the research and development of sensors with high sensitivity and *** this study,a straightforward strategy was proposed for synthesizing ultra-thin oxygen-rich graphitized carbon nanosheets(denoted as GCS-O).These nanosheets are obtained by calcining a topologically two-dimensional indium-based coordination ***,the growth of FeNi Prussian blue analogue(PBA)on GCS-O effectively introduces active sites and increases the nitrogen content within the carbonaceous *** resulting FeNi-PBA/GCS-O composite exhibits excellent glucose sensing performance with a broad linear range of 1 to 1300μmol·L^(-1).Meanwhile,it also achieves a high sensitivity of 2496μA·mmol^(-1)·L·cm^(-2),a limit of detection of 100nmol·L^(-1)(S/N=3),and commendable long-term *** relatively simple synthesis process,exceptional sensitivity,and satisfactory electrochemical sensing performance of FeNi-PBA/GCS-O open up new directions for biosensor applications.

关键词： Coordination polymer Carbon nanosheet Prussian blue analogue Surface reconstruction Glucose oxidation

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