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学者姓名：徐峰
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Abstract ：
Pt/C, as the commonly used electrocatalyst in direct methanol fuel cells, suffers from the difficulty of easy corrosion of the carbon support, which results in a poor catalyst durability in the methanol oxidation reaction (MOR) and oxygen reduction reaction (ORR) processes. The SiO2-CeO2 composite oxide is explored as the noncarbon support to load the PtCu catalyst. PtCu/SiO2-CeO2 with the nanotube morphology exhibited a specific activity (SA) 10.55 times higher than that of Pt/C toward MOR and an SA 3.33 times higher than that of Pt/C toward ORR. Moreover, PtCu/SiO2-CeO2 shows excellent ORR durability, and the activity became even better after 50,000 cycles. The high performance is due to the synergetic effect of SiO2 and CeO2. CeO2 causes an impurity level within SiO2, which alters the electronic structure and the interaction with PtCu. On the other hand, SiO2 imposes a confinement effect on CeO2 and prevents the aggregation of CeO2 nanoparticles which bind PtCu strongly. The density functional theory calculations reveal that the OOH* adsorption of the PtCu/SiO2-CeO2 structure is further enhanced under the synergistic action, leading to a lower overpotential.
Keyword ：
methanol oxidation reaction methanol oxidation reaction noncarbon support noncarbon support oxygen reduction reaction oxygen reduction reaction SiO2-CeO2 SiO2-CeO2 synergetic effect synergetic effect
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| GB/T 7714 | Yang, Liu , Li, Yingrong , Zou, Tianhua et al. Synergetic Effect of SiO2 and CeO2 as the Noncarbon Composite Support on Significantly Promoting Methanol Oxidation and Oxygen Reduction Reaction [J]. | ACS APPLIED ENGINEERING MATERIALS , 2024 , 2 (1) : 170-178 . |
| MLA | Yang, Liu et al. "Synergetic Effect of SiO2 and CeO2 as the Noncarbon Composite Support on Significantly Promoting Methanol Oxidation and Oxygen Reduction Reaction" . | ACS APPLIED ENGINEERING MATERIALS 2 . 1 (2024) : 170-178 . |
| APA | Yang, Liu , Li, Yingrong , Zou, Tianhua , Xu, Feng . Synergetic Effect of SiO2 and CeO2 as the Noncarbon Composite Support on Significantly Promoting Methanol Oxidation and Oxygen Reduction Reaction . | ACS APPLIED ENGINEERING MATERIALS , 2024 , 2 (1) , 170-178 . |
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A direct methanol fuel cell (DMFC) is a promising environmentally friendly energy device, owing to its low emission and high efficiency. Pt/C is the highly efficient catalyst for DMFCs, but Pt is a precious metal, and its weak interaction with a carbon support undermines the structure stability and activity. Herein, two-dimensional ultra-thin cerium oxide (2D-CeO2) was explored as a non-carbon support of the PtCu alloy catalyst for enhancing the electrocatalytic performance towards methanol oxidation (MOR) and oxygen reaction (ORR) reactions. The carbon-free PtCu/2D-CeO2 catalysts show much better electro-activity and durability. Pt0.25Cu/2D-CeO2 exhibits the highest current density of 29.94 mA cm−2 toward the MOR, and a comparable activity to PtCu/C towards the ORR. The exceptional properties, combined with the two-dimensional ultra-thin structure and high column of oxygen vacancies of CeO2, make the PtCu nanoparticles more evenly distributed and more active, significantly improving the activity and durability for the MOR and ORR. © 2024 The Royal Society of Chemistry.
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| GB/T 7714 | Li, Y. , Xu, Z. , Guo, X. et al. An ultra-thin 2D-CeO2 non-carbon support for significantly improving the methanol oxidation and oxygen reduction reactions [J]. | New Journal of Chemistry , 2024 , 48 (31) : 14013-14020 . |
| MLA | Li, Y. et al. "An ultra-thin 2D-CeO2 non-carbon support for significantly improving the methanol oxidation and oxygen reduction reactions" . | New Journal of Chemistry 48 . 31 (2024) : 14013-14020 . |
| APA | Li, Y. , Xu, Z. , Guo, X. , Xu, F. . An ultra-thin 2D-CeO2 non-carbon support for significantly improving the methanol oxidation and oxygen reduction reactions . | New Journal of Chemistry , 2024 , 48 (31) , 14013-14020 . |
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Abstract ：
Pt shows excellent catalytic activity and acid stability towards the methanol oxidation reaction (MOR) and oxygen reduction reaction (ORR), but suffers from deactivation due to the weak interaction with the carbon support and the oxidation of carbon under operation. To solve the problem, herein, silica nanospheres were used to load PtCu nanoparticles as the carbon-free catalyst for the MOR and ORR. It is found that the heat treatment is crucial to regulate the metal-support interaction and enhance the catalytic performance. The PtCu/SiO2 catalyst after heat treatment exhibits a specific activity (SA) nearly 7 times the value of Pt/C toward the MOR, and much better durability. The MOR mass activity of heat-treated PtCu/SiO2 is over twice the value of the untreated one. The electron transfer promoted by heat treatment leads to an upshift of the d-band center of Pt, resulting in the increase of the absorption rate of methanol and the intermediates. © 2023 RSC.
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| GB/T 7714 | Zhao, Q. , Zhi, H. , Yang, L. et al. The heat-promoted metal-support interaction of a PtCu/SiO2 carbon-free catalyst for the methanol oxidation and oxygen reduction reactions [J]. | RSC Sustainability , 2023 , 1 (8) : 1989-1994 . |
| MLA | Zhao, Q. et al. "The heat-promoted metal-support interaction of a PtCu/SiO2 carbon-free catalyst for the methanol oxidation and oxygen reduction reactions" . | RSC Sustainability 1 . 8 (2023) : 1989-1994 . |
| APA | Zhao, Q. , Zhi, H. , Yang, L. , Xu, F. . The heat-promoted metal-support interaction of a PtCu/SiO2 carbon-free catalyst for the methanol oxidation and oxygen reduction reactions . | RSC Sustainability , 2023 , 1 (8) , 1989-1994 . |
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Standardized Precipitation Index (SPI) and Standardized Precipitation Evapotranspiration Index (SPEI), traditionally derived at a monthly scale, are widely used drought indices. To overcome temporal-resolution limitations, we have previously developed and published a well-validated daily SPI/SPEI in situ dataset. Although having a high temporal resolution, this in situ dataset presents low spatial resolu-tion due to the scarcity of stations. Therefore, based on the China Meteorological Forcing Dataset, which is composed of data from more than 1,000 ground-based observation sites and multiple remote sensing grid meteorological dataset, we present the first high spatiotemporal-resolution daily SPI/SPEI raster datasets over China. It spans from 1979 to 2018, with a spatial resolution of 0.1 degrees x 0.1 degrees, a temporal resolution of 1-day, and the timescales of 30-, 90-, and 360-days. Results show that the spatial distributions of drought event characteristics detected by the daily SPI/SPEI are con-sistent with the monthly SPI/SPEI. The correlation between the daily value of the 12-month scale and the monthly value of SPI/SPEI is the strongest, with linear correlation, Nash-Sutcliffe coefficient, and nor-malized root mean square error of 0.98, 0.15, and 0.32, respectively. The daily SPI/SPEI is shown to be more sensitive to flash drought than the monthly SPI/SPEI. Our improved SPI/SPEI shows high accuracy and credibility, presenting enhanced results when compared to the monthly SPI/SPEI. The total data volume is up to 150 GB, compressed to 91 GB in Network Common Data Form (NetCDF). It can be available from Figshare (https://doi.org/10.6084/m9.figshare.c.5823533) and ScienceDB (https://doi.org/10.57760/sciencedb.j00076.00103).
Keyword ：
climate change climate change climatic disaster climatic disaster Drought index Drought index Generalized Extreme Value Generalized Extreme Value
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| GB/T 7714 | Zhang, Rongrong , Bento, Virgilio A. , Qi, Junyu et al. The first high spatial resolution multi-scale daily SPI and SPEI raster dataset for drought monitoring and evaluating over China from 1979 to 2018 [J]. | BIG EARTH DATA , 2023 , 7 (3) : 860-885 . |
| MLA | Zhang, Rongrong et al. "The first high spatial resolution multi-scale daily SPI and SPEI raster dataset for drought monitoring and evaluating over China from 1979 to 2018" . | BIG EARTH DATA 7 . 3 (2023) : 860-885 . |
| APA | Zhang, Rongrong , Bento, Virgilio A. , Qi, Junyu , Xu, Feng , Wu, Jianjun , Qiu, Jianxiu et al. The first high spatial resolution multi-scale daily SPI and SPEI raster dataset for drought monitoring and evaluating over China from 1979 to 2018 . | BIG EARTH DATA , 2023 , 7 (3) , 860-885 . |
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Platinum (Pt) and Pt-based alloys have been extensively studied as efficient catalysts for both the anode and cathode of direct methanol fuel cells (DMFC). Defect engineering has been revealed to be practicable in tuning the charge transfer between Pt and transition metals/supports, which leads to the charge density rearrangement and facilitates the electrocatalytic performance. Herein, Pr-doped CeO2 nanocubes were used as the noncarbon support of a PtCu catalyst. The concentration and structure of oxygen vacancy (V-o) defects were engineered by Pr doping. Besides the V-o monomer, the oxygen vacancy with a linear structure is also observed, leading to the one-dimensional PtCu. The V-o concentration shows the volcanic scenario as Pr increased. Accordingly, the activities of PtCu/PrxCe1-xO2 toward methanol oxidation and oxygen reduction reactions exhibit the volcanic scenario. PtCu/Pr0.15Ce0.85O2 exhibits the optimal catalytic performance with the specific activity 3.57 times higher than that of Pt/C toward MOR and 1.34 times higher toward ORR. The MOR and ORR mass activities of PtCu/Pr0.15Ce0.85O2 reached 1.05 and 0.12 Amg(-1), which are 3.09 and 0.92 times the values of Pt/C, respectively. The abundant V-o afforded surplus electrons, which tailored the electron transfer between PtCu and PrxCe1-xO2, leading to enhanced catalytic performance of PtCu/PrxCe1-xO2. DFT calculations on PtCu/Pr0.15Ce0.85O2 revealed that Pr doping reduced the band gap of CeO2 and lowered the overpotential.
Keyword ：
carbon-freecatalyst carbon-freecatalyst chargetransfer chargetransfer defect engineering defect engineering methanol oxidation methanol oxidation oxygen reduction reaction oxygen reduction reaction
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| GB/T 7714 | Zou, Tianhua , Wang, Yifen , Xu, Feng . Defect-Engineered Charge Transfer in a PtCu/Pr x Ce1-x O2 Carbon-Free Catalyst for Promoting the Methanol Oxidation and Oxygen Reduction Reactions [J]. | ACS APPLIED MATERIALS & INTERFACES , 2023 , 15 (50) : 58296-58308 . |
| MLA | Zou, Tianhua et al. "Defect-Engineered Charge Transfer in a PtCu/Pr x Ce1-x O2 Carbon-Free Catalyst for Promoting the Methanol Oxidation and Oxygen Reduction Reactions" . | ACS APPLIED MATERIALS & INTERFACES 15 . 50 (2023) : 58296-58308 . |
| APA | Zou, Tianhua , Wang, Yifen , Xu, Feng . Defect-Engineered Charge Transfer in a PtCu/Pr x Ce1-x O2 Carbon-Free Catalyst for Promoting the Methanol Oxidation and Oxygen Reduction Reactions . | ACS APPLIED MATERIALS & INTERFACES , 2023 , 15 (50) , 58296-58308 . |
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Abstract ：
本发明属于质子交换膜燃料电池阳极制备技术领域，具体涉及一种二维多孔形貌的二氧化硅非碳载体负载铂铜镍催化剂的制备方法及其应用，本发明是用化学还原法和置换法制备铜镍氢氧化物纳米片作为模板的同时又作为第二和第三金属引入以促进铂催化剂的催化性能，再将二氧化硅包覆在铜镍化合物表面，又经过还原处理成铜镍合金并又均匀且紧密的负载在二氧化硅纳米片的表面，接下来置换载铂，形成铂铜镍合金，最后酸洗获得二维多孔形貌的二氧化硅非碳载体负载铂铜镍催化剂。本发明制备成本低，原料简单且储量丰富，与传统的商业铂碳催化剂相比有着更优异的MOR电催化性能，符合绿色经济和可持续发展理念。
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| GB/T 7714 | 徐峰 , 余晨铭 . 一种二维多孔形貌的二氧化硅非碳载体负载铂铜镍催化剂的制备方法 : CN202111183298.0[P]. | 2021-10-11 00:00:00 . |
| MLA | 徐峰 et al. "一种二维多孔形貌的二氧化硅非碳载体负载铂铜镍催化剂的制备方法" : CN202111183298.0. | 2021-10-11 00:00:00 . |
| APA | 徐峰 , 余晨铭 . 一种二维多孔形貌的二氧化硅非碳载体负载铂铜镍催化剂的制备方法 : CN202111183298.0. | 2021-10-11 00:00:00 . |
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The origin of distinguished oxygen evolution reaction (OER) catalytic properties of multi-principal element alloys (MPEAs) is not clear yet due to the rich surface-active sites may exist in MPEAs composed of multiple types of elements, which may bring complex catalytic environment. In this work, four main steps were carried out using computational materials science. The atom distribution of bulk MPEAs was constructed firstly based on the previously predicted site preference of atoms occupying sublattices, which is beyond the traditional hypothesis that the atom distributing randomly on the whole lattice. Then the (111) close-packed surface slab of CoFeGaNiZn MPEA was obtained by cleaving the bulk structure. Subsequently, the OER processes were systematically explored by calculating the free energy change of intermediates *OH, *O, and *OOH at 171 adsorption sites on the (111) surface. Finally, the oxygen evolution reaction catalytic mechanism and its site preference behavior of FCC_CoFeGaNiZn MPEA were discussed in detail. The results show that atoms have obvious site preference, which deviating the ideal randomly distribution, especially Co, Fe and Zn atoms always prefer to 3c sublattice at all temperature, Ga atoms tend to favor 1a sublattice, and the site preferences of Ni atoms and Ga atoms are affected by the heat treatment temperature. At 1273 K, the site occupying configuration is (Co0.0246Fe0.01680Ga0.4550Ni0.4990Zn0.0046)1a (Co0.2580Fe0.2610Ga0.1150Ni0.1000Zn0.2650)3c. The (111) surface of FCC_CoFeGaNiZn MPEA was based on the site occupying configuration at 1273 K, and it was then supposed to quenched to ground state to simulate the experimental status in the available literature. Since *O at hollow sites transforms into *OOH at a higher overpotential, hollow sites may be poisoning surface sites. Three intermediates are found to primarily participate in the catalytic reaction on top sites. In addition, there are no scaling relationships between Delta E*OH and Delta E*O for CoFeGaNiZn MPEA, even for the same type of top sites. It is noteworthy that an average overpotential of 0.349 V was predicted by considering the combinations of three intermediate-tendency elements, which is in better agreement with the experimental overpotential of 0.37 V at 10 mA/cm2 current density than the overpotential of 0.28 V based on the special quasirandom structures (SQS). Current intensive explorations bring new insights into the OER catalytic mechanism of the preferred adsorption sites of MPEAs based on the reasonable consideration concerning the atoms distributing configuration involving the exact site preference of the constituent metallic atoms on the sublattice.
Keyword ：
Catalytic mechanism Catalytic mechanism Computational materials science Computational materials science Multi -principal element alloys (MPEAs) Multi -principal element alloys (MPEAs) Oxygen evolution reaction (OER) Oxygen evolution reaction (OER) Scaling relationships Scaling relationships Site preference Site preference
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| GB/T 7714 | Weng, Liangji , Su, Longju , Xu, Nengshen et al. The preferred adsorption sites and catalytic mechanism of FCC_CoFeGaNiZn multi-principal element alloy for oxygen evolution reaction catalysis based on site preference of constituent atom on sublattice [J]. | INTERMETALLICS , 2023 , 165 . |
| MLA | Weng, Liangji et al. "The preferred adsorption sites and catalytic mechanism of FCC_CoFeGaNiZn multi-principal element alloy for oxygen evolution reaction catalysis based on site preference of constituent atom on sublattice" . | INTERMETALLICS 165 (2023) . |
| APA | Weng, Liangji , Su, Longju , Xu, Nengshen , Qian, Cheng , Cai, Qi , Chen, Rong et al. The preferred adsorption sites and catalytic mechanism of FCC_CoFeGaNiZn multi-principal element alloy for oxygen evolution reaction catalysis based on site preference of constituent atom on sublattice . | INTERMETALLICS , 2023 , 165 . |
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Pt shows excellent catalytic activity and acid stability towards the methanol oxidation reaction (MOR) and oxygen reduction reaction (ORR), but suffers from deactivation due to the weak interaction with the carbon support and the oxidation of carbon under operation. To solve the problem, herein, silica nanospheres were used to load PtCu nanoparticles as the carbon-free catalyst for the MOR and ORR. It is found that the heat treatment is crucial to regulate the metal-support interaction and enhance the catalytic performance. The PtCu/SiO2 catalyst after heat treatment exhibits a specific activity (SA) nearly 7 times the value of Pt/C toward the MOR, and much better durability. The MOR mass activity of heat-treated PtCu/SiO2 is over twice the value of the untreated one. The electron transfer promoted by heat treatment leads to an upshift of the d-band center of Pt, resulting in the increase of the absorption rate of methanol and the intermediates.
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| GB/T 7714 | Zhao, Quanqing , Zhi, Han , Yang, Liu et al. The heat-promoted metal-support interaction of a PtCu/SiO2 carbon-free catalyst for the methanol oxidation and oxygen reduction reactions [J]. | RSC SUSTAINABILITY , 2023 , 1 (8) : 1989-1994 . |
| MLA | Zhao, Quanqing et al. "The heat-promoted metal-support interaction of a PtCu/SiO2 carbon-free catalyst for the methanol oxidation and oxygen reduction reactions" . | RSC SUSTAINABILITY 1 . 8 (2023) : 1989-1994 . |
| APA | Zhao, Quanqing , Zhi, Han , Yang, Liu , Xu, Feng . The heat-promoted metal-support interaction of a PtCu/SiO2 carbon-free catalyst for the methanol oxidation and oxygen reduction reactions . | RSC SUSTAINABILITY , 2023 , 1 (8) , 1989-1994 . |
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Platinum (Pt), as a commonly used electrocatalyst in direct methanol fuel cells (DMFCs), suffers from sluggish kinetics of both the methanol oxidation reaction (MOR) and oxygen reduction reaction (ORR). Geometric engineering has been proven effective for improving the MOR and ORR activities. Thus, by modulating the Pt precursor and poly(vinylpyrrolidone) (PVP) dosages, different porous PtCu nanotubes constructed by hollow nanospheres, solid alloy, and Pt-rich skinned nanoparticles, respectively, are successfully synthesized. Among them, the solid PtCu alloy nanoparticle coherent nanotubes exhibit the specific activity 9.42 times higher than Pt/C toward MOR, while the hollow PtCu alloy nanosphere coherent nanotubes show the specific activity 4.85 times higher than Pt/C toward ORR. The different Pt:Cu ratios of hollow nanospheres, solid alloy, and Pt-rich skinned nanoparticles cause the differences in electron transfer from Cu to Pt as well as electronic structures of Pt. As a result, the binding energies of intermediates can be regulated, leading to the enhancement in MOR and ORR.
Keyword ：
hollow nanospheres hollow nanospheres methanol oxidation reaction methanol oxidation reaction oxygen reduction reaction oxygen reduction reaction Pt-rich skinned nanoparticles Pt-rich skinned nanoparticles solid alloy nanoparticles solid alloy nanoparticles
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| GB/T 7714 | Xu, Feng , Cai, Shaobin , Lin, Benfeng et al. Geometric Engineering of Porous PtCu Nanotubes with Ultrahigh Methanol Oxidation and Oxygen Reduction Capability [J]. | SMALL , 2022 , 18 (17) . |
| MLA | Xu, Feng et al. "Geometric Engineering of Porous PtCu Nanotubes with Ultrahigh Methanol Oxidation and Oxygen Reduction Capability" . | SMALL 18 . 17 (2022) . |
| APA | Xu, Feng , Cai, Shaobin , Lin, Benfeng , Yang, Liu , Le, Huafeng , Mu, Shichun . Geometric Engineering of Porous PtCu Nanotubes with Ultrahigh Methanol Oxidation and Oxygen Reduction Capability . | SMALL , 2022 , 18 (17) . |
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The widely studied Pt/C catalyst for direct methanol fuel cells (DMFCs) suffers severe carbon corrosion under operation, which undermines the catalytic activity and durability. It is of great importance to develop a carbon-free support with co-catalytic functionality for improving both the activity and durability of Pt-based catalysts. The direct loading of Pt on the smooth surface of oxides may be difficult. Herein, the Cu assisted loading of Pt on CeO2 is developed. Cu pre-coated CeO2 was facilely synthesized and Pt was electrochemically deposited to fabricate the carbon-free PtCu/CeO2 catalyst. The PtCu/CeO2 catalyst has a mass activity up to 1.84 and 1.57 times higher than Pt/C towards methanol oxidation reaction (MOR) and oxygen reduction reaction (ORR), respectively. Better durability is also confirmed by chronoamperometry and accelerated degradation tests. The strategy in this work would be greatly helpful for developing an efficient carbon-free support of Pt-based catalysts for applications in DMFCs.
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| GB/T 7714 | Zou, Linchi , Pan, Jian , Xu, Feng et al. Cu assisted loading of Pt on CeO2 as a carbon-free catalyst for methanol and oxygen reduction reaction [J]. | RSC ADVANCES , 2021 , 11 (58) : 36726-36733 . |
| MLA | Zou, Linchi et al. "Cu assisted loading of Pt on CeO2 as a carbon-free catalyst for methanol and oxygen reduction reaction" . | RSC ADVANCES 11 . 58 (2021) : 36726-36733 . |
| APA | Zou, Linchi , Pan, Jian , Xu, Feng , Chen, Junfeng . Cu assisted loading of Pt on CeO2 as a carbon-free catalyst for methanol and oxygen reduction reaction . | RSC ADVANCES , 2021 , 11 (58) , 36726-36733 . |
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