MOLECULES
·
2023
·Vol. 28
·期 5
·2189
·
IF 4.6
Yunqing Zhu,Bingqing Li,Yongming Wang,Tian Wang
Electrocatalytic oxidation (ECO) has attracted attention because of its high efficiency and environmental friendliness in water treatment. The preparation of anodes with high catalytic activity and long service lifetimes is a core part of electrocatalytic oxidation technology. Here, porous Ti/RuO2-IrO2@Pt, Ti/RuO2-TiO2@Pt, and Ti/Y2O3-RuO2-TiO2@Pt anodes were fabricated by means of modified micro-emulsion and vacuum impregnation methods with high porosity titanium plates as substrates. The scanning electron microscopy (SEM) images showed that RuO2-IrO2@Pt, RuO2-TiO2@Pt, and Y2O3-RuO2-TiO2@Pt nanoparticles were coated on the inner surface of the as-prepared anodes to form the active layer. Electrochemical analysis revealed that the high porosity substrate could result in a large electrochemically active area, and a long service life (60 h at 2 A cm−2current density, 1 mol L−1H2SO4as the electrolyte, and 40 °C). The degradation experiments conducted on tetracycline hydrochloride (TC) showed that the porous Ti/Y2O3-RuO2-TiO2@Pt had the highest degradation efficiency for tetracycline, reaching 100% removal in 10 min with the lowest energy consumption of 167 kWh kg−1TOC. The reaction was consistent with the pseudo-primary kinetics results with a k value of 0.5480 mol L−1s−1, which was 16 times higher than that of the commercial Ti/RuO2-IrO2electrode. The fluorospectrophotometry studies verified that the degradation and mineralization of tetracycline were mainly ascribed to the •OH generated in the electrocatalytic oxidation process. This study thus presents a series of alternative anodes for future industrial wastewater treatment.
研究领域:
环境科学
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材料科学
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产品关联
DOI
PubMed
高影响因子
Catalysts
·
2015
·Vol. 5
·期 2
·606-633
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IF 2
Hongmei Qin,Xiaoshuang Qian,Tao Meng,Yi Lin,Zhen Ma
Conventional supported Pt catalysts have often been prepared by loading Pt onto commercial supports, such as SiO2, TiO2, Al2O3, and carbon. These catalysts usually have simple metal-support (i.e., Pt-SiO2) interfaces. To tune the catalytic performance of supported Pt catalysts, it is desirable to modify the metal-support interfaces by incorporating an oxide additive into the catalyst formula. Here we prepared three series of metal oxide-modified Pt catalysts (i.e., Pt/MOx/SiO2, Pt/MOx/TiO2, and Pt/MOx/Al2O3, where M = Al, Fe, Co, Cu, Zn, Ba, La) for CO oxidation. Among them, Pt/CoOx/SiO2, Pt/CoOx/TiO2, and Pt/CoOx/Al2O3showed the highest catalytic activities. Relevant samples were characterized by N2adsorption-desorption, X-ray diffraction (XRD), transmission electron microscopy (TEM), H2temperature-programmed reduction (H2-TPR), X-ray photoelectron spectroscopy (XPS), CO temperature-programmed desorption (CO-TPD), O2temperature-programmed desorption (O2-TPD), and CO2temperature-programmed desorption (CO2-TPD).Keywords:Pt catalysts;cobalt oxide;CO oxidation
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Nature Catalysis
·
2022
·Vol. 5
·期 6
·503-512
·
IF 40.706
Xiao Fei,Wang Qi,Xu Gui-Liang,Qin Xueping,Hwang Inhui,Sun Cheng-Jun,Liu Min,Hua Wei,Wu Hsi-wen,Zhu Shangqian,Li Jin-Cheng,Wang Jian-Gan,Zhu Yuanmin,Wu Duojie,Wei Zidong,Gu Meng,Amine Khalil,Shao Minhua
Proton exchange membrane fuel cells convert hydrogen and oxygen into electricity without emissions. The high cost and low durability of Pt-based electrocatalysts for the oxygen reduction reaction hinder their wide application, and the development of non-precious metal electrocatalysts is limited by their low performance. Here we design a hybrid electrocatalyst that consists of atomically dispersed Pt and Fe single atoms and Pt–Fe alloy nanoparticles. Its Pt mass activity is 3.7 times higher than that of commercial Pt/C in a fuel cell. More importantly, the fuel cell with a low Pt loading in the cathode (0.015 mg Pt cm −2 ) shows an excellent durability, with a 97% activity retention after 100,000 cycles and no noticeable current drop at 0.6 V for over 200 hours. These results highlight the importance of the synergistic effects among active sites in hybrid electrocatalysts and provide an alternative way to design more active and durable low-Pt electrocatalysts for electrochemical devices.
研究领域:
材料科学
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电化学
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能源技术
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2023
·Vol. 14
·期 1
·1-10
·
IF 16.6
Jin Hui,Xu Zhewei,Hu Zhi-Yi,Yin Zhiwen,Wang Zhao,Deng Zhao,Wei Ping,Feng Shihao,Dong Shunhong,Liu Jinfeng,Luo Sicheng,Qiu Zhaodong,Zhou Liang,Mai Liqiang,Su Bao-Lian,Zhao Dongyuan,Liu Yong
The design of Pt-based nanoarchitectures with controllable compositions and morphologies is necessary to enhance their electrocatalytic activity. Herein, we report a rational design and synthesis of anisotropic mesoporous Pt@Pt-skin Pt 3 Ni core-shell framework nanowires for high-efficient electrocatalysis. The catalyst has a uniform core-shell structure with an ultrathin atomic-jagged Pt nanowire core and a mesoporous Pt-skin Pt 3 Ni framework shell, possessing high electrocatalytic activity, stability and Pt utilisation efficiency. For the oxygen reduction reaction, the anisotropic mesoporous Pt@Pt-skin Pt 3 Ni core-shell framework nanowires demonstrated exceptional mass and specific activities of 6.69 A/mg pt and 8.42 mA/cm 2 (at 0.9 V versus reversible hydrogen electrode), and the catalyst exhibited high stability with negligible activity decay after 50,000 cycles. The mesoporous Pt@Pt-skin Pt 3 Ni core-shell framework nanowire configuration combines the advantages of three-dimensional open mesopore molecular accessibility and compressive Pt-skin surface strains, which results in more catalytically active sites and weakened chemisorption of oxygenated species, thus boosting its catalytic activity and stability towards electrocatalysis.
研究领域:
材料科学
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电化学
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纳米技术
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催化
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2021
·
IF 3.764
Hailin Zhao,Bingjing Tang,Jie Tang,Yafeng Cai,Yao Cui,Hao Liu,Li Wang,Yunsong Wang,Wangcheng Zhan,Yanglong Guo,Yun Guo
Catalytic oxidation is believed to be the most efficient method for indoor formaldehyde purification. Herein, we reported that the Pt/Na-ZSM-5 catalyst with low Pt loading (0.16 wt %) prepared by depositing Pt on Na+ ion-exchanged ZSM-5 could completely oxidize 300 ppm formaldehyde in 2.5 vol % H2O at 32 °C and maintain its activity during the 62 h-long stability test. Multiple characterizations revealed that the presence of Na species significantly enhanced formaldehyde adsorption ability and made Pt species tend to exist in the form of metal Pt through electron transfer from Na to Pt, which promoted the activation of oxygen and opened a new efficient formaldehyde oxidation pathway, namely, direct decomposition of formate. The synergistic effects resulted in the TOF of Pt(0.16)/Na-ZSM-5 being about nine times higher than that of Pt(0.50)/ZSM-5. Our study showed that utilizing an alkali metal to tune the surface acidity/basicity of the support and the state of the supported noble metal was a promising way to improve the intrinsic catalytic performance and reduce noble metal usage.
研究领域:
环境科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2024
·
IF 10.8
Wei Chen,Juan Zheng,Yarong Fang,Yutao Wang,Jinpeng Hu,Yuhua Zhu,Xiaoxiao Zhu,Weihao Li,Qian Zhang,Chuanqi Pan,Baojian Zhang,Xiaofeng Qiu,Sibo Wang,Shuang Cui,Jinlong Wang,Jinsong Wu,Zhu Luo,Yanbing Guo
Typically, SO2 unavoidably deactivates catalysts in most heterogeneous catalytic oxidations. However, for Pt-based catalysts, SO2 exhibits an extraordinary boosting effect in propane catalytic oxidation, but the promotive mechanism remains contentious. In this study, an in situ-formed tactful (Pt–S–O)-Ti structure was concluded to be a key factor for Pt/TiO2 catalysts with a substantial SO2 tolerance ability. The experiments and theoretical calculations confirm that the high degree of hybridization and orbital coupling between Pt 5d and S 3p orbitals enable more charge transfer from Pt to S species, thus forming the (Pt–S–O)-Ti structure with the oxygen atom dissociated from the chemisorbed O2 adsorbed on oxygen vacancies. The active oxygen atom in the (Pt–S–O)-Ti active structure is a robust site for C3H8 adsorption, leading to a better C3H8 combustion performance. This work can provide insights into the rational design of chemical bonds for high SO2 tolerance catalysts, thereby improving economic and environmental benefits.
研究领域:
催化化学
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环境科学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2021
·
IF 4.311
Zhongliang Huang,Yujia Yuan,Miaomiao Song,Zhimian Hao,Jingran Xiao,Dongren Cai,Abdul-Rauf Ibrahim,Guowu Zhan
Herein, we fabricated a series of bimetallic Pt-Ni catalysts supported on mesoporous silica nanorods ( m SNR, specific BET surface area of 1802 m 2 g −1 ) to study the effect of Ni/Pt ratio on the product selectivity in CO 2 hydrogenation. Both monometallic Pt/ m SNR and Ni 50 Pt 50 / m SNR catalysts revealed negligible methane selectivity. However, methane became the major product only when increasing the Ni/Pt ratio up to 9. X-ray photoelectron spectroscopy (XPS) and inductively coupled plasma (ICP) characterizations showed that the Pt/Ni ratio on the catalyst surface was appreciably higher than the bulk composition, suggesting the enrichment of Pt on the surface ( e.g. , Pt/Ni of 61/39 for Ni 50 Pt 50 / m SNR catalyst). The Pt/Ni ratio was crucial in determining the CH 4 /CO selectivity, and the addition of a tiny amount of Pt could improve the catalytic performance and stability of Ni/ m SNR. Among the different catalysts, Ni 98 Pt 2 / m SNR showed the best CO 2 conversion (59%) and CH 4 selectivity (96%) at 400 °C, 0.1 MPa, 9600 mL h −1 g cat −1 , and H 2 /CO 2 of 3. In-situ DRIFTS and temperature-programmed surface experiments suggested that the dissociated adsorption of CO 2 on the Pt site led to CO*, but the strongly adsorbed CO* cannot be further hydrogenated to CH 4 over the Pt site. In contrast, CO* could be further hydrogenated into CH 4 via CH x O* intermediates on adjacent Ni sites.
研究领域:
催化
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材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2019
·
IF 7.723
Jian Zhou,Junhui Hu,Xueqiong Zhang,Jiefei Li,Kunhong Jiang,Yajun Liu,Guohui Zhao,Xiaojing Wang,Haibin Chu
Using nanocrystals with specific crystal facets is an effective way to enhance activity and selectivity for numerous catalytic reactions . However, the intrinsic facet effect is not fully understood. Herein, using Pt catalyzed glycerol oxidation reaction as the model system, the intrinsic facet effect on catalytic property is evaluated by three kinds of Pt nanocrystal catalysts with cubic, spherical and tetrahedral shapes. Size effect, support effect, surfactant effect as well as the metal-support interaction of the catalysts are avoided to the maximum extent. The supported Pt nanocubes enclosed by Pt(1 0 0) facets are found to exhibit much higher catalytic activity and stability for the aerobic oxidation of glycerol than catalysts with Pt nanotetrahedrons enclosed by Pt(1 1 1) facets. DFT calculations indicate that the adsorption of oxygen and glycerol would materialize easier on Pt(1 0 0) than on Pt(1 1 1). Furthermore, Pt(1 0 0) may prevent deactivation caused by product adsorption as well.
研究领域:
催化
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材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
Nature Energy
·
2021
·Vol. 6
·期 6
·614-623
·
IF 60.858
Gao Ruijie,Wang Jian,Huang Zhen-Feng,Zhang Rongrong,Wang Wei,Pan Lun,Zhang Junfeng,Zhu Weikang,Zhang Xiangwen,Shi Chengxiang,Lim Jongwoo,Zou Ji-Jun
Platinum is the archetypal electrocatalyst for oxygen reduction—a key reaction in fuel cells and zinc–air batteries. Although dispersing platinum as single atoms on a support is a promising way to minimize the amount required, catalytic activity and selectivity are often low due to unfavourable O 2 adsorption. Here we load platinum onto α-Fe 2 O 3 to construct a highly active and stable catalyst with dispersed Pt–Fe pair sites. We propose that the Pt–Fe pair sites have partially occupied orbitals driven by strong electronic coupling, and can cooperatively adsorb O 2 and dissociate the O=O bond, whereas OH* can desorb from the platinum site. In alkaline conditions, the catalyst exhibits onset and half-wave potentials of 1.15 V and 1.05 V (versus the reversible hydrogen electrode), respectively, mass activity of 14.9 A mg −1 Pt (at 0.95 V) and negligible activity decay after 50,000 cycles. It also shows better performance than 20% Pt/C in a zinc–air battery and H 2 –O 2 fuel cell in terms of specific energy density and platinum utilization efficiency.
研究领域:
催化
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电化学
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材料科学
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能源存储与转换
✓ 已验证
DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-12
·
IF 14.7
Zhang Tengfei,Zheng Peng,Gao Jiajian,Liu Xiaolong,Ji Yongjun,Tian Junbo,Zou Yang,Sun Zhiyi,Hu Qiao,Chen Guokang,Chen Wenxing,Liu Xi,Zhong Ziyi,Xu Guangwen,Zhu Tingyu,Su Fabing
Developing high-performance Pt-based catalysts with low Pt loading is crucial but challenging for CO oxidation at temperatures below 100 °C. Herein, we report a Pt-based catalyst with only a 0.15 wt% Pt loading, which consists of Pt–Ti intermetallic single-atom alloy (ISAA) and Pt nanoparticles (NP) co-supported on a defective TiO 2 support, achieving a record high turnover frequency of 11.59 s –1 at 80 °C and complete conversion of CO at 120 °C. This is because the coexistence of Pt–Ti ISAA and Pt NP significantly alleviates the competitive adsorption of CO and O 2 , enhancing the activation of O 2 . Furthermore, Pt single atom sites are stabilized by Pt–Ti ISAA, resulting in distortion of the TiO 2 lattice within Pt–Ti ISAA. This distortion activates the neighboring surface lattice oxygen, allowing for the simultaneous occurrence of the Mars-van Krevelen and Langmuir–Hinshelwood reaction paths at low temperatures.
研究领域:
催化
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化学工程
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Catalysis Science & Technology
·
2015
·Vol. 6
·期 7
·2403-2412
·
IF 5.426
Dong Wang,Yujun Zhu,Chungui Tian,Lei Wang,Wei Zhou,Yongli Dong,Qing Han,Yunfei Liu,Fulong Yuan,Honggang Fu
The introduction of a suitable co-catalyst is a promising way to improve the catalytic efficiency of Pt catalysts. Herein, SBA-15 modified with well-dispersed Mo2N nanoparticles (NPs) is synthesized by anchoring phosphomolybdic acid (HPM) on aminated SBA-15 (SBA-15-NH2) primarily, followed by nitridation treatment under NH3. After loading of Pt, the Pt–Mo2N/SBA-15 catalyst with close-contact Pt and Mo2N NPs can be formed. The intensive interaction of Pt and Mo2N benefited from the close contact is verified by XRD and XPS tests. As a result, the ternary Pt–Mo2N/SBA-15 catalysts have shown superior performance to Pt/SBA-15 catalysts for the selective hydrogenation of cinnamaldehyde to cinnamyl alcohol. The TOF over the 1 wt% Pt–Mo2N/SBA-15 catalyst is close to that over the 3 wt% Pt/SBA-15 catalyst, but its selectivity to cinnamyl alcohol (COL) is 2.5 times that of 3 wt% Pt/SBA-15. The promoted activity of Pt–Mo2N/SBA-15 is mainly attributed to the synergistic effect of Pt and Mo2N NPs, which can cause the full development of the catalytic ability of Pt, thus reducing the Pt usage, through increasing the dispersion of Pt NPs and the fraction of Pt0 species in the catalyst.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2018
·
IF 5.091
Jiabai Cai,Xueqing Wu,Yuehai Li,Ye Lin,Hui Yang,Shunxing Li
The goal of this work was to assess the performance of Pt nanoparticles (NPs) as co-catalysts on the photocatalytic activity of TiO 2 @Pt@C 3 N 4 hollow spheres, which was tested by photodegrading rhodamine B and methyl blue under visible light irradiation. TiO 2 @Pt@C 3 N 4 composites were fabricated by using modified polystyrene balls as templates, hydrothermal reactions , and calcination . Under simulated sunlight irradiation, photocatalytic activity was in the following of TiO 2 @Pt@C 3 N 4 > TiO 2 @C 3 N 4 > C 3 N 4 > P25. The photo-conversion rate of the TiO 2 @Pt@C 3 N 4 increased significantly relative to TiO 2 @C 3 N 4 and the others. The combination of TiO 2 and C 3 N 4 , as well as the sandwiched of Pt NPs reduce electron-hole recombination as a result of having an electron trap site, which can store and shuttle photo-generated electrons, and enhance photo-generation of active radicals. Electron paramagnetic resonance (EPR) spectroscopy, as well as photo-luminescence (PL), and electrochemical measurements were taken to verify this conclusion. Considering the multi-functional combination of precious metals and semiconductor materials , this work may provide new ideas for the design of high-performance catalysts.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）