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Enhanced Thermoelectric Performance of Non-equilibrium Synthesized Fe0.4Co3.6Sb12-xGex Skutterudites via Randomly Distributed Multi-scaled Impurity Dots

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Journal of Wuhan University of technology(materials Science) 2018年第4期33卷 772-777页

作者：章嵩 HU Xuan 杨梅君 CHENG Hong TU Rong ZHANG Lianmeng State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China The Center for Materials Research and Analysis Wuhan University of TechnologyWuhan 430070China

The p-type Ge doped Fe0.4Co3.6Sb12-xGex skutterudites with multi-scaled impurity dots（500 nm-2 mm） were successfully prepared by using melt-quenching（MQ） and subsequent spark plasma sintering（SPS） technique. Compared with traditional method, the new technology significantly shortened the processing time from several days to less than 24 hours. The phase of impurity dots was demonstrated to be CoSb through analysis of X-ray diffraction（XRD） and energy-dispersive spectrum（EDS）. Impurity dots were induced by Ge substitution of Sb in the non-equilibrium synthesized process. Due to the abandonment of the long reaction of annealing crystallization, a few of Ge atoms would fail to substitute Sb site of skutterudite in this non-equilibrium synthesized process, leading to that the multi-scaled impurity dots randomly distributed in the matrix of skutterudite Fe0.4Co3.6Sb12-xGex. The combination of multi-scaled impurity dots scattering long wavelength heat-carrying phonons and the point defect scattering short and middle wavelength heat-carrying phonons dramatically made the 22.2% reduction of lattice thermal conductivity. As a result, compared with unsubstituted sample of Fe0.4Co3.6Sb12, the maximum ZT value was increased by 30.5%. Thus, the two marked features of this new synthesis process, the shortened preparation time and the enhanced thermoelectric performance, would make a promising commercial application in the future.

关键词： multi-scaled impurity dots Sb site substitution p-type thermoelectric transport properties

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Bismuth oxide nanoflake@carbon film: A free-standing battery-type electrode for aqueous sodium ion hybrid supercapacitors

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Chinese Chemical Letters 2018年第4期29卷 629-632页

作者： Zhenshuai Zhao Yihua Ye Weihua Zhu Liang Xiao Bohua Deng Jinping Liu School of Chemistry Chemical Engineering and Life Science Wuhan University of Technology State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology

Aqueous hybrid supercapacitors are promising due to their low cost and high safety. Herein, a freestanding battery-type electrode of Bi2O3 nanoflake@C on carbon cloth is designed for aqueous sodium ion hybrid supercapacitors. Due to the integration of nanoarray architecture and the conductive carbon,the Bi2O3@C electrode exhibits a high specific capacity of 207 mAh/g at 2 A/g（6C）, good rate capability and cycling stability（133 m Ah/g after 1000 cycles）. With the activated carbon as the capacitive electrode and neutral sodium salts as the electrolyte, a 1.9 V hybrid supercapacitor is assembled,delivering a high energy density of 18.94 Wh/kg. The device can still maintain 72.3% of initial capacity after 650 cycles. The present work holds great promise for developing next-generation hybrid supercapacitors.

关键词： Bi2O3 film Free-standing Carbon hybridization Hybrid supercapacitors

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Low-Cost Hydroxyacid Potassium Synergists as an Efficient In Situ Defect Passivator for High Performance Tin-Oxide-Based Perovskite Solar Cells

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Angewandte Chemie 2023年第25期135卷

作者： Wei Dong Chenpu Zhu Cong Bai Yue Ma Linfeng Lv Juan Zhao Fuzhi Huang Yi-Bing Cheng Jie Zhong Research Centre for Advanced Thin Film Photovoltaics State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 P. R. China Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory Foshan 528216 Guangdong Province P. R. China School of Automobile Engineering Wuhan University of Technology Wuhan 430070 P. R. China

Perovskite solar cells (PSCs) based on SnO 2 electron transport layers have attracted extensive research due to their compelling photovoltaic performance. Herein, we presented an in situ passivation of SnO 2 with low-cost hydroxyacid potassium synergist during deposition to optimize the interface carrier extraction and transport for high power conversion efficiency (PCE) and stabilities of PSCs. The orbital overlap of the carboxyl oxygen with the Sn atom alongwith the homogenous nano-particle deposition effectively suppresses the interfacial defects and releases the internal residual strains in the perovskite. Accordingly, a PCE of 24.91 % with a fill factor (FF) up to 0.852 is obtained for in situ passivated devices, which is one of the highest values for SnO 2 -based PSCs. Moreover, the unencapsulated device maintained 80 % of its initial PCE at 80 °C over 600 h, 100 % PCE at ambient conditions for 1300 h, and 98 % after one week maximum power point tracking (MPPT) under continuous AM1.5G illumination.

关键词： Chemical Bath Deposition Defect Passivation Electron Transport Layer Perovskite Solar Cells

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Boosting Electrocatalytic Nitrogen Reduction on Cobalt-Based Perovskite via Regulating Reaction Pathway Through Donation-Back-Donation Modulation

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Angewandte Chemie 2025年第25期137卷

作者： Ning Han Wei Zhang Jianxiang Wu Kaibin Chu Shihui Feng Shuo Wang Alain R. Puente-Santiago Jinlin Long Bo Weng Bao-Lian Su The Edward S. Rogers Department of Electrical and Computer Engineering University of Toronto Ontario ON M5S 1A4 Canada These authors are cofirst authors. Institute of Energy Materials Science University of Shanghai for Science and Technology Shanghai 200093 China Shanghai Key Laboratory of Materials Protection and Advanced Materials Electric Power Shanghai University of Electric Power Shanghai 200090 China School of Materials Science and Engineering Linyi University Linyi 276000 China Department of Materials and Environmental Chemistry Arrhenius Laboratory Stockholm University Stockholm 10 691 Sweden State Key Laboratory of Chemistry for NBC Hazards Protection State Key Laboratory of Photocatalysis on Energy and Environment College of Chemistry Fuzhou University Fuzhou 350116 China Department of Chemistry and Biochemistry Florida International University Miami FL USA State Key Laboratory of Advanced Environmental Technology Institute of Urban Environment Chinese Academy of Sciences Xiamen 361021 China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 China Laboratory of Inorganic Materials Chemistry (CMI) University of Namur 61 rue de Bruxelles Namur 5000 Belgium

The electrocatalytic approach of combining N 2 and H 2 O to produce ammonia, known as the electrocatalytic N 2 reduction reaction (eNRR), has garnered significant attention due to its environmental benefits and potential for supporting a decentralized agricultural economy. However, the underlying chemistry governing the reaction pathways remains poorly understood, hindering the design of low-cost and efficient eNRR catalysts. Here we report the enhancement of the electrocatalytic eNRR activity of perovskite oxides by tuning the reaction pathway through a “donation-back-donation” mechanism. This is achieved by controlling the spin state via adjusting the distribution of d orbital electrons in low-cost transition metals, such as cobalt. Specifically, the cobalt in perovskite SrCoO 3 (SC) with a low-spin state demonstrates an 18 times higher ammonia yield rate compared to that in Co 3 O 4 and 1.5 times higher than cobalt in perovskite LaCoO 3 (LC). The low spin states of cobalt in SC enable better control of the eNRR reaction pathway over the transformation of *N 2 H to *NHNH or *NNH 2 , resulting in alternating hydrogenation in SC rather than distal hydrogenation in LC with a high spin state. The unprecedented improvement in eNRR by regulating the spin state of Co demonstrates the bright of low-cost Co-based electrocatalysts for ammonia production.

关键词： D orbital electron distribution Nitrogen reduction reaction Perovskite Reaction pathway Regulation of spin state

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Intermediate phase-enhanced Ostwald ripening for the elimination of phase segregation in efficient inorganic CsPbIBr_(2)perovskite solar cells

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Science China materials 2021年第11期64卷 2655-2666页

作者： Wei Li Benjia Zhu Mathias Uller Rothmann Amelia Liu Weijian Chen Yen Yee Choo Narendra Pai Wenxin Mao Tian Zhang Qiaoliang Bao Xiaoming Wen Udo Bach Joanne Etheridge Yi-Bing Cheng Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory Xianhu hydrogen ValleyFoshan 528200China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China Department of Physics University of OxfordOxford OX13PUUnited Kingdom School of Physics and Astronomy Monash UniversityVictoria 3800Australia Centre for Micro-Photonics Swinburne University of TechnologyHawthorn 3122Australia Australian Research Council Centre of Excellence in Exciton Science Monash UniversityVictoria 3800Australia Department of Materials Science and Engineering Monash UniversityVictoria 3800Australia Department of Chemical Engineering Monash UniversityVictoria 3800Australia Commonwealth Scientific and Industrial Research Organization Manufacturing FlagshipClaytonVictoria 3168Australia Melbourne Centre for Nano fabrication 151 Wellington RoadClaytonVIC 3168Australia Monash Centre for Electron Microscopy Monash UniversityVictoria 3800Australia

Mixed halide perovskites with the ability to tune bandgaps exhibit attractive applications in tandem solar cells,building integrated photovoltaic and wavelength-tunable light-emitting ***,halide demixing under illumination or in the dark with a charge-carrier injection in both hybrid and inorganic perovskites results in bandgap instability and current-density-voltage(J-V)hysteresis,which can significantly hamper their ***,we demonstrate that halide segregation and J-V hysteresis in mixed halide inorganic CsPbIBr_(2)solar cells can be effectively mitigated by introducing an intermediate phase-enhanced Ostwald ripening through the control of the chemical composition in the CsPbIBr_(2)precursor *** amounts of either PbBr_(2)or CsI are incorporated into originally even molar amounts of PbBr_(2)and CsI precursor *** the PbBr_(2)-excess,we observed an enlarged perovskite grain size,no detectable halide phase segregation at the grain boundaries nor the perovskite/TiO2 interface,an increased minority carrier lifetime,a reduced J-V hysteresis,and an improved solar-cell ***,different CsI:PbBr_(2)stoichiometric ratios were found to have different effects on the performance of the perovskite solar *** excessive lead phase is reactive with the dimethyl sulfoxide(DMSO)in the precursor solution to form the Pb(I,Br)2·DMSO complex and the quasi-twodimensional(2D)CsPb_(2)(I,Br)5,which are conducive to Ostwald maturation and defect ***,the CsPbIBr_(2)solar cell with a PbBr_(2)-excess precursor composition reaches a power conversion efficiency(PCE)of 9.37%(stabilized PCE of 8.48%)and a maximum external quantum efficiency of over 90%.

关键词： solar cells phase segregation CsPbIBr_(2) cathodoluminescence transmission electron microscope

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Liquid Fluxional Ga Single Atom Catalysts for Efficient Electrochemical CO2Reduction

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Angewandte Chemie 2022年第3期135卷

作者： Dr. Zedong Zhang Jiexin Zhu Dr. Shenghua Chen Prof. Wenming Sun Prof. Dingsheng Wang Department of Chemistry Tsinghua University Beijing 100084 China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 Hubei China Department of Chemistry Beijing Key Laboratory for Optical Materials and Photonic Devices Capital Normal University Beijing 100048 China

Precise design and tuning of the micro-atomic structure of single atom catalysts (SACs) can help efficiently adapt complex catalytic systems. Herein, we inventively found that when the active center of the main group element gallium (Ga) is downsized to the atomic level, whose characteristic has significant differences from conventional bulk and rigid Ga catalysts. The Ga SACs with a P, S atomic coordination environment display specific flow properties, showing CO products with FE of ≈92 % at −0.3 V vs. RHE in electrochemical CO 2 reduction (CO 2 RR). Theoretical simulations demonstrate that the adaptive dynamic transition of Ga optimizes the adsorption energy of the *COOH intermediate and renews the active sites in time, leading to excellent CO 2 RR selectivity and stability. This liquid single atom catalysts system with dynamic interfaces lays the foundation for future exploration of synthesis and catalysis.

关键词： CO2RR Fluxional Single Atom Catalysts Liquid Metal Ga

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Abatement of Emissions of a Residential Wood Stove: Effect of the Catalyst on Gaseous and Condensable Pollutants Concentration and Their Toxicity

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ACS Omega 2025年第24期10卷 25506-25517页

作者： Marvin Laboureur Maxence Hannard Tarek Barakat Abhishek Goel Jordi Cornette Svend Bram Patricia Renard Thomas Duquesne Bao-Lian Su Laboratory of Inorganic Materials Chemistry (CMI) − Namur Institute of Structured Matter (NISM) University of Namur rue de Bruxelles 61 Namur 5000 Belgium；Stuv S.A. Rue Riverre 10-12 Floreffe 5150 Belgium Laboratory of Inorganic Materials Chemistry (CMI) − Namur Institute of Structured Matter (NISM) University of Namur rue de Bruxelles 61 Namur 5000 Belgium；Empa - Swiss Federal Laboratories for Materials Science and Technology Ueberlandstrasse 129 Dübendorf 8600 Switzerland Thermo and Fluid Dynamics (FLOW) Vrije Universiteit Brussel (VUB) Pleinlaan 2 Brussels 1050 Belgium；Brussels Institute for Thermal-fluid Systems and Clean Energy (BRITE) Vrije Universiteit Brussel (VUB) and Université Libre de Bruxelles (ULB) Brussels 1050 Belgium Thermo and Fluid Dynamics (FLOW) Vrije Universiteit Brussel (VUB) Pleinlaan 2 Brussels 1050 Belgium；Brussels Institute for Thermal-fluid Systems and Clean Energy (BRITE) Vrije Universiteit Brussel (VUB) and Université Libre de Bruxelles (ULB) Brussels 1050 Belgium；Faculty of Aerospace Engineering Delft University of Technology Kluyverweg 1 Delft 2629 HS The Netherlands Laboratory of Biochemistry and Cell Biology (URBC)-Namur Research Institute for Life Sciences (NARILIS) University of Namur Rue de Bruxelles 61 Namur 5000 Belgium Stuv S.A. Rue Riverre 10-12 Floreffe 5150 Belgium Laboratory of Inorganic Materials Chemistry (CMI) − Namur Institute of Structured Matter (NISM) University of Namur rue de Bruxelles 61 Namur 5000 Belgium；State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology 122 Hongshan Luoshi Road Wuhan 430070 China

The use of biomass combustion for residential heating purposes is crucial for reaching the European Union’s 2050 climate-neutrality goals. It, however, raises environmental and health concerns. This study explores the impact of a patented catalyst on wood stove emissions and, notably, its influence on cytotoxicity by comparing flue gas composition with and without the catalyst. Organic gaseous compounds (OGC) generated by wood combustion comprise two subgroups: water-soluble condensable organic compounds (WSCOC) and high-saturating vapor organic compounds (HSVOC). The second is mainly composed of methane, a molecule challenging to oxidize into CO2at these operating temperatures. While the catalyst moderately eliminates OGC (19%) in general, it excels in removing CO (87%) and WSCOC (80%), particularly polycyclic aromatic hydrocarbons (PAH) (91%). Bioassays on the A549 human cell line show that the catalytic WSCOC removal is correlated with a significant decrease in cytotoxicity (50%). Additionally, particle number size distribution measurements suggest that the catalyst facilitates the deposition of particles larger than 10 μm, leading to a 66% reduction in the particulate mass concentration. These results underscore the catalyst’s role in mitigating harmful gaseous emissions and reducing the health risks associated with wood stove use, particularly by targeting toxic WSCOC.

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High-Entropy Lithium Argyrodite Solid Electrolytes Enabling Stable All-Solid-state Batteries

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Angewandte Chemie 2023年第50期135卷

作者： Shenghao Li Jing Lin Mareen Schaller Sylvio Indris Xin Zhang Torsten Brezesinski Ce-Wen Nan Shuo Wang Florian Strauss Center of Smart Materials and Devices State Key Laboratory of Advanced Technology for Materials Synthesis and Processing & School of Material Science and Engineering Wuhan University of Technology Wuhan 430070 China Institute of Nanotechnology Karlsruhe Institute of Technology (KIT) Hermann-von-Helmholtz-Platz 1 76344 Eggenstein-Leopoldshafen Germany Institute for Applied Materials-Energy Storage Systems (IAM-ESS) Karlsruhe Institute of Technology (KIT) Hermann-von-Helmholtz-Platz 1 76344 Eggenstein-Leopoldshafen Germany State Key Laboratory of New Ceramics and Fine Processing School of Materials Science and Engineering Tsinghua University Beijing 100084 China Foshan (Southern China) Institute for New Materials Foshan 528200 China

Superionic solid electrolytes (SEs) are essential for bulk-type solid-state battery (SSB) applications. Multicomponent SEs are recently attracting attention for their favorable charge-transport properties, however a thorough understanding of how configurational entropy (Δ S conf ) affects ionic conductivity is lacking. Here, we successfully synthesized a series of halogen-rich lithium argyrodites with the general formula Li 5.5 PS 4.5 Cl x Br 1.5- x (0≤ x ≤1.5). Using neutron powder diffraction and 31 P magic-angle spinning nuclear magnetic resonance spectroscopy, the S 2− /Cl − /Br − occupancy on the anion sublattice was quantitatively analyzed. We show that disorder positively affects Li-ion dynamics, leading to a room-temperature ionic conductivity of 22.7 mS cm −1 (9.6 mS cm −1 in cold-pressed state) for Li 5.5 PS 4.5 Cl 0.8 Br 0.7 (Δ S conf =1.98 R ). To the best of our knowledge, this is the first experimental evidence that configurational entropy of the anion sublattice correlates with ion mobility. Our results indicate the possibility of improving ionic conductivity in ceramic ion conductors by tailoring the degree of compositional complexity. Moreover, the Li 5.5 PS 4.5 Cl 0.8 Br 0.7 SE allowed for stable cycling of single-crystal LiNi 0.9 Co 0.06 Mn 0.04 O 2 (s-NCM90) composite cathodes in SSB cells, emphasizing that dual-substituted lithium argyrodites hold great promise in enabling high-performance electrochemical energy storage.

关键词： Argyrodite High-Entropy materials Solid Electrolyte Solid-state Batteries

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A TiSe 2 -Graphite Dual Ion Battery: Fast Na-Ion Insertion and Excellent Stability

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Angewandte Chemie (International ed. in English) 2021年第34期60卷 18430-18437页

作者： Runtian Zheng Haoxiang Yu Xikun Zhang Yang Ding Maoting Xia Kangzhe Cao Jie Shu Alexandru Vlad Bao-Lian Su School of Materials Science and Chemical Engineering Ningbo University Ningbo 315211 Zhejiang China. Laboratory of Inorganic Materials Chemistry (CMI) University of Namur 61 rue de Bruxelles 5000 Namur Belgium. State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 Hubei China. Henan Province Key Laboratory of Utilization of Non-Metallic Mineral in the South of Henan Xinyang Normal University Xinyang 464000 Henan China. Institute of Condensed Matter and Nanosciences Université Catholique de Louvain Place Louis Pasteur 1L4.01.02 1348 Louvain-la-Neuve Belgium.

The sodium dual ion battery (Na-DIB) technology is proposed as highly promising alternative over lithium-ion batteries for the stationary electrochemical energy-storage devices. However, the sluggish reaction kinetics of anode materials seriously impedes their practical implementation. Herein, a Na-DIB based on TiSe -graphite is reported. The high diffusion coefficient of Na-ions (3.21×10 -1.20×10 cm s ) and the very low Na-ion diffusion barrier (0.50 eV) lead to very fast electrode kinetics, alike in conventional surface capacitive storage systems. In-situ investigations reveal that the fast Na-ion diffusion involves four insertion stage compositions. A prototype cell shows a reversible capacity of 81.8 mAh g at current density of 100 mA g , excellent stability with 83.52 % capacity retention over 200 cycles and excellent rate performance, suggesting its potential for next-generation large scale high-performance stationary energy storage systems.

关键词： TiSe2 dual-ion batteries graphite cathodes reaction mechanisms sodium

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无模板法合成具有增强催化活性的分级纳米孔结构MIL-101(Cr)

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中国科学：材料科学（英文版） 2021年第1期64卷 252-258页

作者：赵田李松贺肖宇轩 Christoph Janiak 常刚刚田歌阳晓宇 State Key Laboratory of Advanced Technology for Materials Synthesis and Processing & School of Materials Science and Engineering & School of Chemistry Chemical Engineering and Life Science Wuhan University of Technology Wuhan 430070 China Key Laboratory of Advanced Packaging Materials and Technology of Hunan Province School of Packaging and Materials Engineering Hunan University of Technology Zhuzhou 412007 China Institut für Anorganische Chemie und Strukturchemie Universität Düsseldorf Universitätsstr. 1 D-40225 Düsseldorf Germany Southern Marine Science and Engineering Guangdong Laboratory (Zhuhai) & School of Chemical Engineering and Technology Sun Yat-sen University Zhuhai 519000 China School of Engineering and Applied Sciences Harvard University Cambridge Massachusetts 02138 USA

MIL-101(Cr)是最重要的金属有机框架(MOFs)材料之一,稳定的框架结构和超高的比表面积使其在众多科学领域得到了广泛研究和应用.但是MIL-101(Cr)的合成条件比较苛刻,且稳定性较强,因此,有关于其分级结构的研究报道仍比较少.本文提出了一... 详细信息

MIL-101(Cr)是最重要的金属有机框架(MOFs)材料之一,稳定的框架结构和超高的比表面积使其在众多科学领域得到了广泛研究和应用.但是MIL-101(Cr)的合成条件比较苛刻,且稳定性较强,因此,有关于其分级结构的研究报道仍比较少.本文提出了一种简单制备分级纳米孔结构MIL-101(Cr)的方法,即以乙酸作为调节剂,采用水热合成的方法,一步得到具有微孔-介孔-大孔分级结构的MIL-101(Cr)材料.实验结果表明,该分级结构的MIL-101(Cr)与无分级结构的MIL-101(Cr)相比,其大分子染料吸附能力和催化能力均有显著提高.而且分级结构MIL-101(Cr)负载了磷钨酸催化剂之后,表现出了与均相催化剂(纯磷钨酸)相当的催化能力.进一步研究发现,使用其他短碳链的一元羧酸作为调节剂,如丙酸、丁酸等,也可获得类似分级纳米结构MIL-101(Cr).

关键词： Template-free synthesis micro-meso-macroporous hierarchy MIL-101(Cr)

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