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Rationally construction of atomic-precise interfacial charge transfer channel and strong build-in electric field in nanocluster-based Zscheme heterojunctions with enhanced photocatalytic hydrogen production

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Nano Research 2024年第6期17卷 5002-5010页

作者： Qingtao Zhu Honglei Shen Chao Han Liu Huang Yanting Zhou Yuanxin Du Xi Kang Manzhou Zhu Department of materials Science and Engineering Centre for Atomic Engineering of Advanced MaterialsKey Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of EducationKey Laboratory of Functional Inorganic Material Chemistry of Anhui ProvinceAnhui UniversityHefei 230601China

The lack of effective charge transfer driving force and channel limits the electron directional migration in nanoclusters(NC)-based heterostructures,resulting in poor photocatalytic ***,a Z-scheme NC-based heterojunction(Pt1Ag28-BTT/CoP,BTT=1,3,5-benzenetrithiol)with strong internal electric field is constructed via interfacial Co-S bond,which exhibits an absolutely superiority in photocatalytic performance with 24.89 mmol·h^(−1)·g−1 H_(2)production rate,25.77%apparent quantum yield at 420 nm,and~100%activity retention in stability,compared with Pt1Ag28-BDT/CoP(BDT=1,3-benzenedithiol),Ag29-BDT/CoP,and *** enhanced catalytic performance is contributed by the dual modulation strategy of inner core and outer shell of NC,wherein,the center Pt single atom doping regulates the band structure of NC to match well with CoP,builds internal electric field,and then drives photogenerated electrons steering;the accurate surface S modification promotes the formation of Co-S atomic-precise interface channel for further high-efficient Z-scheme charge directional *** work opens a new avenue for designing NC-based heterojunction with matchable band structure and valid interfacial charge transfer.

关键词： atomically precise metal nanocluster Z-scheme heterojunction interfacial charge transfer build-in electric field photocatalytic hydrogen production

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Hierarchical porous(Ta_(0.2)Nb_(0.2)Ti_(0.2)Zr_(0.2)Hf_(0.2))C high-entropy ceramics prepared by a self-foaming method for thermal insulation

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Journal of Advanced Ceramics 2024年第7期13卷 956-966页

作者： Cuiyan Li Ruinan Gao Haibo Ouyang Tianzhan Shen Zihao Chen Yanlei Li key laboratory for Green Manufacturing&functional Application of inorganic materials School of Materials Science and EngineeringShaanxi University of Science and TechnologyXi’an 710021China

To meet the emerging demands for thermal protection materials for hypersonic aircraft,developing porous ultrahigh-temperature ceramics with both robust mechanical properties and superior thermal insulation performance is a critical ***,we report novel porous(Ta_(0.2)Nb_(0.2)Ti_(0.2)Zr_(0.2)Hf_(0.2))C high-entropy carbide(PHEC)ceramics fabricated by a self-foaming method using commercially available metal chloride and furfuryl alcohol(FA)as *** PHEC ceramics are constructed of microspheres with a size of 2µm,leading to a high porosity of 91.3%and an interconnected *** microspheres consist of high-entropy carbide grains(20 nm),resulting in abundant interfaces and nanosized pores in the PHEC *** to its unique hierarchical structure,the prepared PHEC ceramics have outstanding compressive strength(28.1±2 MPa)and exceptionally low thermal conductivity(κT,0.046 W·m^(-1)·K^(-1))at room *** makes it a promising thermal insulation materials for ultrahigh temperature *** work provides a cost-effective and facile strategy for producing porous ultrahigh-temperature ceramics.

关键词： porous ceramics high-entropy carbides hierarchical structure thermal insulation self-foaming

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Energy transfer, anticounterfeiting, white light emission and sensing in fine-regulating series of lanthanide metal-organic frameworks

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Journal of Rare Earths 2024年第3期42卷 446-454,I0001页

作者： Juanjuan Xue Yao Wang Guoping Yang Yaoyu Wang key laboratory of Synthetic and Natural functional Molecule Chemistry of the Ministry of Education Shaanxi Key Laboratory of Physico-Inorganic ChemistryCollege of Chemistry&Materials ScienceNorthwest UniversityXi'an710127China

Three lanthanide ions and a rigid(1,1'-biphenyl)-2,4,6-tricarboxylic acid(H_(3)bptc) ligand led to the isostructural lanthanide metal-organic frameworks(Ln-MOFs) {[Ln(bptc)(H_(2)O)_(3)]·3H_(2)O}_n(Lnbptc, Ln = Eu,Tb, Gd, Eu_(x)Tb_(1—x), Eu_(x)Gd_(1-x), Tb_(x)Gd_(1-x), and Eu_(0.12)Tb_(0.52)Gd_(0.36)). The density functional theory(DFT) and time-dependent DFT calculation were expanded on H_3bptc, which point to the occurrence of “antenna effect”. The minor diameter samples of Eubptc, Tbbptc, and Gdbptc can also be attained via the microwave synthesis and employed for handwriting anticounterfeiting. Interestingly, the typical red emission of Eu^(3+) and green emission of Tb~(3+) could be fine-tuned by Gd^(3+) via chemical mixing to be full-color emissions bimetallic doped Eu_(x)Tb_(1-x)bptc, Eu_(x)Gd_(1-x)bptc, and Tb_(x)Gd_(1-x)bptc. The above synthetic bimetallic MOFs can be fixed in positioning boxes of quick response(QR) codes with diverse emission for anticounterfeiting. The message can be decoded under the irradiation of 365 nm ultraviolet lamp while invisible in the daylight. Notably, the trimetallic doped Eu_(0.12)Tb_(0.52)Gd_(0.36)bptc emits white light with the CIE color coordinate(0.34, 0.34). Furthermore, Tbbptc is demonstrated to be a sensitive probe toward nitrobenzene and acetone with multiple mechanisms.

关键词： Metal-organic frameworks Anticounterfeiting White light-emitting Sensing Rare earths

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β-C(sp^(3))−H chlorination of amide derivatives via photoinduced copper charge transfer catalysis

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Chinese Chemical Letters 2024年第2期35卷 361-365页

作者： Yuhang He Chao Tian Guanghui An Guangming Li key laboratory of functional inorganic Material Chemistry (MOE) School of Chemistry and Materials ScienceHeilongjiang UniversityHarbin 150080China

An atom economicβ-C(sp^(3))−H chlorination of amide derivatives has been *** mild protocol employs CuCl_(2) instead of palladium catalysts with atom-economic HCl as chlorine sources and enables the late-stage functionalization of medicine *** studies suggest a plausible visible light triggered ligand-to-metal charge transfer(LMCT)/1,4-hydrogen atom transfer(HAT)cascade.

关键词： Photoinduced copper catalysis Ligand-to-metal charge transfer 1,4-Hydrogen atom transfer β-Halogenated amide Late-stage functionalization

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Well-dispersed Sb particles embedded on N-doped carbon nanofibers toward high-performance Li-ion battery

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Rare Metals 2024年第7期43卷 2994-3006页

作者： Ying Li Yi-Han Zhao Lu-Lu Zhao Peng-Fei Wang Ying Xie Ting-Feng Yi School of materials Science and Engineering Northeastern UniversityShenyang 110819China key laboratory of Dielectric and Electrolyte functional Material Hebei Province School of Resources and MaterialsNortheastern University at QinhuangdaoQinhuangdao 066004China key laboratory of functional inorganic Material Chemistry Ministry of EducationSchool of Chemistry and Materials ScienceHeilongjiang UniversityHarbin 150080China

The alloy-type material Sb is widely used in the anode materials of lithium-ion batteries(LIBs)due to its high theoretical specific ***,its serious volume expansion problem during alloying/dealloying of Li~+limits its practical *** this work,C-Sb composite was constructed as anode material of LIBs by electrospinning route for the first time,Sb was introduced into the polyacrylonitrile-based hard carbon and coal tar pitch-based soft carbon composite amorphous carbon fiber with a diameter of 300-600 nm,which realized high cycling *** C-Sb-2(the mass ratio of polyacrylonitrile to Sb source is 1:2)electrode displayed charge capacities of 1098.5,930.3,841.7,753.5,643.9 and 545.8 mAh·g^(-1)at 0.1,0.2,0.3,0.5,1 and 2 A·g^(-1),*** when the current density returned to 0.1 A·g^(-1),the charge capacity was 939.3 mAh·g^(-1),revealing good stability and *** introduction of Sb into the amorphous carbon improved its conductivity and addressed the volume expansion issue of high specific capacity Sb during charge/***-situ XRD analysis confirmed the high reversibility of the C-Sb-2 during charging and *** functional theory(DFT)calculations revealed the gradual enhancement of the interface interaction between Sb_(x)Li_(y) and amorphous carbon(AMC)with increasing lithium content,contributing to the anchoring of alloy nanoparticles on the AMC surface and buffering the volume change of the ***,the gradual lithiation of Sb facilitated the electron transfer from Sb_(x)Li_(y) to *** findings hold promise for designing lithium storage materials with exceptional performance,highlighting the potential of C-Sb composites as anode materials for efficient next-generation lithium storage.

关键词： Li-ion battery Metallic Sb Carbon Electrospinning Cycling stability

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General synthesis of transition metal nitride arrays by ultrafast flash Joule heating within 500 ms

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Science China Chemistry 2024年第6期67卷 1976-1982页

作者： Peiqi Shen Jiahui Zhao Yanan Gao Yunxiang Lin Yuchen Han Kun Xu School of Chemistry and Chemical Engineering Key Laboratory of Functional Inorganic Material Chemistry of Anhui ProvinceAnhui Province Key Laboratory of Chemistry for Inorganic/Organic Hybrid Functionalized MaterialsKey Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of EducationAnhui UniversityHefei230601China Institutes of Physical Science and Information Technology Center of Free Electron Laser&High Magnetic FieldLeibniz International Joint Research Center of Materials Sciences of Anhui ProvinceAnhui UniversityHefei230601China

Transition metal nitrides(TMNs)are considered as viable alternatives to noble metal catalysts owing to their versatile electronic structure and favorable catalytic ***,the conventional synthetic processes for TMNs suffer from high energy consumption and low production *** this study,a range of TMNs and their hetero-composite arrays were successfully synthesized via an ultrafast flash Joule heating technology within 0.5 *** a proof concept,the nitrides and hetero-composites were applied for the electrocatalytic hydrazine oxidation reaction(HzOR),in which the Co_(4)N/Mo_(16)N_(7)arrays shows the best performance with a geometric current density of 100 mA cm^(-2)at 23 mV(*** hydrogen electrode(RHE)).This work paves a new way for the ultrafast synthesis of TMNs which could meet the ever-increased energy crisis.

关键词： flash Joule heating rapid synthesis transition metal nitrides hydrazine oxidation reaction electrocatalysts

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A robust indium-organic framework with open tubular channels for efficient separation of acetylene

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Nano Research 2024年第4期17卷 3139-3146页

作者： Yong-Zhi Li Gang-Ding Wang Fan Xu Qing Yin Danyang Zhao Jiqiu Qi Yanwei Sui Lei Hou Yao-Yu Wang School of materials and Physics China University of Mining and TechnologyXuzhou 221116China key laboratory of Synthetic and Natural functional Molecule of the Ministry of Education Shaanxi Key Laboratory of Physico-Inorganic ChemistryCollege of Chemistry&Materials ScienceNorthwest UniversityXi’an 710069China

Considering the tremendous applications and purification requirement of acetylene(C_(2)H_(2)),seeking appropriate adsorbents with high capacity and selectivity is a vital task and remains an enduring ***,we designed and synthesized a robust three-dimensional(3D)indium-organic framework([(Me)_(2)NH_(2)][In(L6)_(0.5)(IPA)_(0.5)]·DMA·2H_(2)O(In-L6-IPA,DMA=dimethylammonium,IPA=isopropyl alcohol))featuring two types of one-dimensional(1D)tubular *** activated In-L6-IPA displayed high loading for C_(2)H_(2)(104.4 cm^(3)·g^(-1),the second highest value among all reported indium-based metal-organic frameworks(MOFs))and simultaneously selective adsorption for C_(2)H_(2) over CO_(2),C_(2)H_(6),and ethylene(C_(2)H_(4))at 298 K under 100 *** modelling revealed that the porous wall of In-L6-IPA provides more and stronger multiple interactions for C_(2)H_(2) than CO_(2),C_(2)H_(6),and C_(2)H_(4) containing C–H···π,C–H···O,and O···π*** experiments validated the actual separation ability for various ratios of binary C_(2)H_(2)/C_(2)H_(4) and C_(2)H_(2)/CO_(2) mixtures as well as equimolar ternary C_(2)H_(2)/C_(2)H_(4)/CO_(2) and C_(2)H_(2)/C_(2)H_(4)/C_(2)H_(6) mixtures with excellent reusability.

关键词： indium-organic framework crystal structure gas adsorption acetylene(C_(2)H_(2))separation

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Tuning interface mechanism of FeCo alloy embedded N,S-codoped carbon substrate for rechargeable Zn-air battery

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Journal of Energy Chemistry 2024年第6期93卷 400-410,I0010页

作者： Hui Chang Lulu Zhao Shan Zhao Zong-Lin Liu Peng-Fei Wang Ying Xie Ting-Feng Yi School of materials Science and Engineering Northeastern UniversityShenyang 110819LiaoningChina key laboratory of functional inorganic Material Chemistry Ministry of EducationSchool of Chemistry and Materials ScienceHeilongjiang UniversityHarbin 150080HeilongjiangChina key laboratory of Dielectric and Electrolyte functional Material Hebei Province School of Resources and MaterialsNortheastern University at QinhuangdaoQinhuangdao 066004HebeiChina

The interface mechanism between catalyst and carbon substrate has been the focus of *** this paper,the FeCo alloy embedded N,S co-doped carbon substrate bifunctional catalyst(FeCo/S-NC)is obtained by a simple one-step pyrolysis *** experimental results and density functional theory(DFT)calculation show that the formation of FeCo alloy is conducive to promoting electron transfer,and the introduction of S atom can enhance the interaction between FeCo alloy and carbon substrate,thus inhibiting the migration and agglomeration of particles on the surface of carbon *** FeCo/SNC catalysts show outstanding performance for oxygen reduction reaction(ORR)and oxygen evolution reaction(OER).FeCo/S-NC shows a high half-wave potential(E_(1/2)=0.8823 V)for ORR and a low overpotential at 10 mA cm^(-2)(E_(j=10)=299 mV)for *** addition,compared with Pt/C+RuO_(2) assembled Zn-air battery(ZAB),the FeCo/S-NC assembled ZAB exhibits a larger power density(198.8 mW cm^(-2)),a higher specific capacity(786.1 mA h g_(zn)~(-1)),and ultra-stable cycle *** results confirm that the optimized composition and the interfacial interaction between catalyst and carbon substrate synergistically enhance the electrochemical performance.

关键词： FeCo alloy N S co-doped carbon DFT calculation Zn-air batteries Interfacial interaction

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Gradient-structure-enhanced dielectric energy storage performance of flexible nanocomposites containing controlled preparation of defective TiO_(2) and ferroelectric KNbO_(3) nanosheets

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Nano Research 2024年第5期17卷 4079-4088页

作者： Yan Wang Lili Zhao Ruicong Chen Wenhui Zhao Dengwei Hu Haoran Wang Bin Cui key laboratory of Synthetic and Natural functional Molecule of the Ministry of Education Shaanxi key laboratory of Physico–inorganic Chemistry Xi’an Key Laboratory of Functional Supramolecular Structure and MaterialsCollege of Chemistry and Materials ScienceNorthwest UniversityXi’an 710127China School of Information Science and Technology Northwest UniversityXi’an 710127China Engineering Research Center for Titanium Based functional materials and Devices in Universities of Shaanxi Province Faculty of Chemistry and Chemical EngineeringBaoji University of Arts and SciencesBaoji 721013China

Next generation power system needs dielectrics with increased dielectric energy ***,the low energy density of dielectrics limits their ***,an asymmetric trilayered nanocomposite,with a transition layer(TL),an insulation layer(IL),and a polarization layer(PL),is designed based on poly(vinylidene fluoride)-polymethyl methacrylate(PVDF-PMMA)matrix using KNbO_(3)(KN)and TiO_(2)(TO)as the *** morphology and defect control of the two-dimensional nano KN and nano TO fillers are realized via a hydrothermal method to increase the composite breakdown strength(E_(b))and the composite energy density(U_(e)).The asymmetric trilayered structure leads to a gradient electric field distribution,and the KN and TO nanosheets block charges transfer along z *** a result,the development path of the electrical trees is greatly curved,and E_(b) is effectively *** the Ue value of the nanocomposites reaches 17.79 J·cm^(-3) at 523 MV·m^(-1).On the basis,the composite Ue is further improved by defect control in TO *** nanocomposite KN/TO/PVDF-PMMA containing TO with less oxygen vacancy concentration(calcined at oxygen atmosphere)acquires a high Ue of 21.61 J·cm^(-3) at 548 MV·m^(-1).This study provides an idea for improving the energy storage performance by combining the design of the composite dielectric structure and the control of nanofillers’defect and morphology.

关键词： asymmetric trilayered structure two-dimensional energy density oxygen vacancies breakdown strength dielectric

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Synergistic Ru/RuO_(2) heterojunctions stabilized by carbon coating as efficient and stable bifunctional electrocatalysts for acidic overall water splitting

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Nano Research 2024年第8期17卷 6931-6939页

作者： Man Wu Yuying Fan Yang Huang Dongxu Wang Ying Xie Aiping Wu Chungui Tian key laboratory of functional inorganic Material Chemistry Ministry of Education of the People’s Republic of ChinaHeilongjiang UniversityHarbin 150080China

The development of highly active and stable acidic water oxidation electrocatalysts is of great significant for promoting the industrial application of proton exchange membrane ***-based catalysts have broad application prospects in acidic water oxidation,but their limitations in stability and activity hinder their further ***,a nitrogen-doped carbon(NC)coated porous Ru/RuO_(2) heterojunctional hollow sphere(Ru/RuO_(2)/NC)is designed as high-active and stable bifunctional electrocatalyst for acidic oxygen evolution reaction(OER)and hydrogen evolution reaction(HER).In synthesis,the key is to use mesoporous polydopamine spheres as a template for forming hollow spheres,a source of NC coating and a reducing agent for forming Ru/RuO_(2) *** Ru/RuO_(2) heterojunction adjusts the electronic structure of Ru active sites,optimizing the adsorption of intermediate ***,the NC coating and the interaction between NC and Ru/RuO_(2) effectively prevent Ru from over-oxidation and *** porous hollow structure provides more exposed active sites and promotes mass ***,Ru/RuO_(2)/NC exhibits outstanding OER and HER performance with low overpotentials of 211 and 32 mV at 10 mA·cm^(−2),respectively,and shows excellent *** acid water splitting electrolyzer,based on the bifunctional Ru/RuO_(2)/NC,requires low cell voltages of 1.46 and 1.76 V at 10 and 100 mA·cm^(−2),respectively,with good stability for over 100 h operation,surpassing Pt/C||RuO_(2) and most of the reported catalysts.

关键词： hollow heterojunction bifunctional electrocatalysts oxygen evolution hydrogen evolution acidic water splitting

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