INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2020
·
IF 4.939
Na Ye,Yanxin Bai,Zhao Jiang,Tao Fang
In the work, the catalytic performance and reaction mechanism of methanol oxidation reaction(MOR) are studied for the bimetallic Pd x Cu y and Pd x Ni y catalysts in alkaline solution. The results reveal that the Pd 1 Ni 1 /C and Pd 1 Cu 1 /C bimetallic catalysts exhibit high catalytic activity 4.1 and 3.9 times higher than that of the commercial Pd/C catalyst. Combined with the X-ray diffraction (XRD), High-resolution transmission electron microscopy(HRTEM) and X-ray photoelectron spectroscopy (XPS) analysis, the charge transfer between Pd and Cu(or Ni) alters the electron density of Pd and enhances the anti-CO poisoning ability, which is confirmed by DFT (Density Functional Theory) calculations. The CO binding energy is weakened on various bimetallic surfaces compared with that on Pd(111), consistent with experimental results. A linear relationship exists between the CO binding energy and the catalytic activity on the bimetallic catalysts, indicating that the CO binding energy may be the potential descriptor for MOR in alkaline media .
研究领域:
催化化学
·
材料科学
·
理论计算
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Rongying Zhu,Yaodong Yu,Renqin Yu,Jianping Lai,Joey Chung-Yen Jung,Shiming Zhang,Yufeng Zhao,Jiujun Zhang,Zhonghong Xia
It remains a huge challenge to develop methanol oxidation electrocatalysts with remarkable catalytic activity and anti-CO poisoning capability. Herein, PtIrNi and PtIrCo jagged nanowires are successfully synthesized via a facile wet-chemical approach. Pt and Ir components are concentrated in the exterior and Ni is concentrated in the interior of PtIrNi jagged nanowires, while PtIrCo jagged nanowires feature the homogeneous distribution of constituent metals. The PtIrNi and PtIrCo jagged nanowires exhibit mass activities of 1.88 A/mg Pt and 1.85 A/mg Pt , respectively, 3.24 and 3.19 times higher than that of commercial Pt/C (0.58 A/mg Pt ). In-situ Fourier transform infrared spectroscopy indicates that CO 2 was formed at a very low potential for both nanowires, in line with the high ratio of forward current density to backward current density for PtIrNi jagged nanowires (1.30) and PtIrCo jagged nanowires (1.46) relative to Pt/C (0.76). Also, the CO stripping and X-ray photoelectron spectroscopy results substantiate the remarkable CO tolerance of the jagged nanowires. Besides, the two jagged nanowires possess exceptional activities toward ethanol and ethylene glycol oxidation reactions. This work provides a novel line of thought in terms of rational design of alcohol oxidation electrocatalysts with distinctive nanostructures .
研究领域:
材料科学
·
电化学
·
纳米技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nano Research
·
2021
·Vol. 14
·期 7
·2441-2450
·
IF 8.897
Peng Lingxin,Tian Han,Cui Xiangzhi,Su Liang,Meng Ge,Ma Zhonghua,Cao Shaowen,Shi Jianlin
Developing anode catalysts of substantially enhanced activity for hydrogen oxidation reaction (HOR) and anti-CO poisoning performance is of great importance for the application of proton exchange membrane fuel cells (PEMFCs). Herein, we report Pd cluster in situ decorated urchin-like W 18 O 49 (WO 2.72 ) electrocatalysts by a photo-reduction method for high performance HOR. The synthesized Pd-WO 2.72 -L composite of low loading amount of 0.44 wt.% Pd by Xenon light reduction exhibits markedly high HOR catalytic activity and stability in 0.5 M H 2 SO 4 , and the specific HOR current density and mass activity of Pd-WO 2.72 -L are ∼ 1.5 and ∼ 80 times those of 20 wt.% Pt/C catalyst, respectively. Moreover, excellent anti-CO poisoning ability has also been obtained. The excellent HOR activity and anti-CO poisoning performance of Pd-WO 2.72 -L have been discussed mainly in terms of the dual synergetic catalytic effects between Pd and WO 2.72 : Pd activation to Pd δ+ by the electron transfer from Pd to W promotes the hydrogen adsorption and activation to H* species, which results in largely elevated HOR activity; Pd degradation due to the CO poisoning is effectively prevented by WO 2.72 , which is responsible for the excellent CO-tolerance performance.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Jiayu Jin,Shuozhen Hu,Xinsheng Zhang,Shigang Sun
Palladium is a promising formic acid electro-oxidation (FAO) catalyst due to its higher initial activity than platinum. However, suffering from the adsorption of hydrogen and CO-like species, the activity and stability of Pd are still unsatisfied. Herein, palladium nanoparticles deposited on carbon supported molybdenum trioxide (Pd–MoO 3 /C) is prepared with MoO 3 as the promoter for FAO. X-ray photoelectron spectroscopy analysis proves the close contact between Pd and MoO 3 , which generates the hydrogen spillover effect and forms the Pd–Mo structure. The hydrogen spillover effect enhances the desorption of hydrogen from Pd and facilitates the FAO activity. Both the spillover effect and Pd–Mo structure contribute to the removal of CO ad and facilitate the durability and anti-CO poisoning ability of the catalyst. With the optimized ratio of MoO 3 to carbon black, the Pd–MoO 3 /C-20 catalyst owns the best specific activity of 5.86 mA cm −2 , which is 1.86 times of Pd/C.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2021
·Vol. 168
·期 5
·052507
·
IF 4.316
Qingchun Wang,Zihao Wang,Xiaolong Liang,Shengli An,Changkun Cai,Yuanyuan Liu,Jinxiao Bao,Xiwen Song
Spherical CeO2 and CeO2-ZrO2 solid solutions are prepared using a hydrothermal method, Pt/CeO2-ZrO2/GO and Pt-CeO2/GO catalysts are prepared using graphene as a carrier, and the effects of the addition of a CeO2-ZrO2 solid solution on the electrocatalytic activity, stability and anti-CO poisoning performance of methanol fuel cell anodes are investigated. The catalyst samples are characterized via X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM) and transmission electron microscopy (TEM), and the electrochemical properties of the catalysts are investigated using an electrochemical workstation (IVIUM). The results show that Pt/CeO2-ZrO2/GO has a higher electrocatalytic activity and stability against CO oxidation than Pt-CeO2/GO, Pt/GO and commercial Pt/C catalysts, which is attributed to ZrO2. When Zr4+ is added into the CeO2 lattice, the activity of oxygen in the CeO2 lattice, the oxygen mobility and the oxygen vacancies are increased, the oxygen storage capacity is improved, and the intermediate product of CO is more easily oxidized. This finding indicates that Pt/CeO2-ZrO2/GO is a methanol oxidation anode catalyst with a good catalytic activity, stability and resistance to CO poisoning.
研究领域:
材料科学
·
电化学
·
能源科学
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Lianjin Chen,Xiaosen Wang,Aimei Zhu,Qiugen Zhang,Qinglin Liu
Direct ethanol fuel cell can convert chemical energy into electric energy directly, and has the advantages of being free from Carnot cycle and being friendly to environment, so it has a broad application prospect. However, the insufficient activity and toxicity resistance of anodic catalysts limit their commercial application, mainly due to the limited adsorption sites and the toxic inactivation of catalysts resulting from the production of toxic intermediates (CO ads ) during the ethanol oxidation reaction (EOR) process. In this study, the Au@PdAg porous hemispherical catalyst assembled by nanotubes was successfully prepared by soft template method and co-reduction method using dioctadecyl dimethyl ammonium chloride (DODAC) as surfactant, and its EOR performance was tested. Au@Pd 1.0 Ag 1.0 has the highest mass current density with a peak value of 4048.8 mA mg Pd − 1 , which is 7.8 times of Pd/C (JM). After 5000 s stability test, the residual current density value is still 863.4 mA mg Pd − 1 . The results showed that the introduction of the oxygenophilic metal Ag was conducive to the formation of OH ads and the oxidation of CO ads . The porous structure of the nanotube assembly facilitates electron transfer and provides more adsorption sites, which makes the catalyst show good electrocatalytic activity and anti-CO poisoning ability.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2019
·Vol. 166
·期 4
·F264
·
IF 3.12
Yuxia Pan,Maomao Tu,Xiaoqin Shi,Qi Zhang,Xiaoyu Guo,Mengzhu Li,Yiping Wu,Ye Ying,Ying Wen,Haifeng Yang
The direct methanol fuel cell calls for designing various highly active catalysts containing less platinum, still keeping with reasonable stability. In this work, through controlling reaction system under acidic media (pH = 1), ∼3 nm PtPd nanoparticles are dispersed onto the TiO2 support (3PtPd/TiO2) via a facile one-pot hydrothermal route. In comparison with that of homemade Pt/TiO2 and commercial Pt black catalysts, as-synthesized 3PtPd/TiO2 shows a better performance for directly electrochemical catalysis of methanol and simultaneously exhibits high ability against poison from carbon oxide species. Clearly, the optimized usage of anatase TiO2 not only enhances catalytic activity due to the metal-support interactions but also improves long durability, which could be attributed to the OH existing at the surfaces of TiO2 and Pd.
研究领域:
材料科学
·
电化学
·
能源科学
✓ 已验证
DOI
高影响因子
MATERIALS RESEARCH BULLETIN
·
2013
·
IF 1.913
Liming Jiang,Honggang Fu,Lei Wang,Guang Mu,Baojiang Jiang,Wei Zhou,Ruihong Wang
Tungsten carbide/porous carbon (WC/PC) composites have been successfully synthesized through a surfactant assisted evaporation-induced-assembly method, followed by a thermal treatment process. In particular, WC/PC-35-1000 composite with tungsten content of 35% synthesized at the carbonized temperature of 1000 °C, exhibited a specific surface area ( S BET ) of 457.92 m 2 g −1 . After loading Pt nanoparticles (NPs), the obtained Pt/WC/PC-35-1000 catalyst exhibits the highest unit mass electroactivity (595.93 A g −1 Pt) toward methanol electro-oxidation, which is about 2.6 times as that of the commercial Pt/C (JM) catalyst. Furthermore, the Pt/WC/PC-35-1000 catalyst displays much stronger resistance to CO poisoning and better durability toward methanol electrooxidation compared with the commercial Pt/C (JM) catalyst. The high electrocatalytic activity, strong poison-resistivity and good stability of Pt/WC/PC-35-1000 catalyst are attributed to the porous structures and high specific surface area of WC/PC support could facilitate the rapid mass transportation. Moreover, synergistic effect between WC and Pt NPs is favorable to the higher catalytic performance.
研究领域:
材料科学
·
电化学
·
催化领域
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2022
·
IF 7.139
Xiaoying Qi,Xiang Gong,Na Ye,Zhao Jiang,Tao Fang
Direct methanol and formic acid fuel cells attracted extensive attention with high specific energy and low operating temperature. The efficient electrocatalyst was one of the important factors to limit their commercial applications. Here, the nitrides-modified Pd/C catalysts (Pd–NbN/C, Pd–Mo 2 N/C, Pd-VN/C and Pd-BN/C) were prepared using sodium citrate as a reducing agent in ethylene glycol solution. The mass activities followed the trend of Pd–NbN/C > Pd–Mo 2 N/C > Pd-VN/C > Pd-BN/C > Pd/C, where Pd–NbN/C exhibited the highest mass activity (4052.19 A g Pd −1 ) for MOR, 19.2 times that of the commercial Pd/C (210.53 A g Pd −1 ). Electrochemical measurements (LSV, Tafel, EIS, CA) indicated that the addition of nitrides increased the charge-transfer kinetics, reaction rate and CO tolerance of catalysts for MOR in alkaline media . The rate-determining step was CO ads oxidation process . Combined the structural analysis (HRTEM, XRD , XPS , ICP) with electrochemical results, the enhanced catalytic performance was ascribed to that higher ECSAs and the charge transfer between Pd and nitrides, leading to the negative shift of the d-band center towards the Fermi level . The linear correlations were found for the d-band center VS the mass activities and the onset potential of CO oxidation VS the d-band center, indicating that the activity and anti-CO poisoning ability could be enhanced by controlling the d-band structure of catalysts for MOR. Furthermore, the higher mass activity for FAOR in acidic media suggested that nitrides-modified Pd/C may be the promising bi-functional materials.
研究领域:
电化学
·
催化材料科学
✓ 已验证
产品关联
DOI
高影响因子
Materials Today Chemistry
·
2022
·
IF 7.613
W. Zhan,L. Ma,M. Gan
Herein, we report an efficient bottom-up approach to construct the carbon encapsulated CoP nanoarray-like architectures onto the nitrogen-doped Ti 3 C 2 MXene Pt-based catalyst (Pt–CoP@CNT NA/N–Ti 3 C 2 ) by employing metal-organic frameworks (MOFs) as the sacrificial template. Benefiting from the catalytic effect for metals into MOFs and synergistic effect of Ti 3 C 2 substrate, homogenous nanotubes nanoarray-like structure is obtained on Ti 3 C 2 nanosheet . The unique heteroatom-doped 3D connected structure endows the catalyst with distinct structural merits, such as the carbon and nitrogen-enriched structures, large specific surface areas and excellent conductivity, leading to the high dispersion of ultrafine metallic Pt and efficient electronic/mass transfer, contributing to more exposed active sites of Pt surface. The fabricated CoP and doped nitrogen especially for those lattice nitrogen derived from the pristine MOFs can present exceptional co-catalytic effect, resulting in obtaining strong anti-CO poisoning capacity for catalyst. Therefore, the ultrahigh catalytic activity of per Pt active site for methanol oxidation reaction can be preserved. Besides, owing to the strong stability of carrier, the catalyst delivers a reliable long-term stability during the test. This work gives new ideal for the design of novel cost-effective 3D Ti 3 C 2 -based nanomaterial catalyst with excellent catalytic activity for methanol oxidation.
研究领域:
材料科学
·
催化化学
·
能源转换与存储
✓ 已验证
产品关联
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2020
·
IF 6.215
Na Ye,Zhao Jiang,Tao Fang
Direct methanol fuel cells (DMFCs) have attracted extensive attention due to clean, efficient characteristics and portable applications. In this work, a series of Pd x Cu y /reduced graphene oxide (rGO) catalysts are assembled and the catalytic performances are investigated for methanol oxidation reaction (MOR) in alkaline media. The intrinsic surface electronic structures of the Pd x Cu y /rGO bimetallic catalysts are also studied to clarify the reaction mechanism. The results reveal that Pd 1.2 Cu 0.2 /rGO exhibits superior catalytic activity (1101.58 A g Pd −1 ), 4.2 and 5.2 times higher than those of the commercial PtRu/C and Pd/C catalysts. CO stripping suggests that the onset potential for CO oxidation on the Pd 1.2 Cu 0.2 /rGO catalyst is lower than those on the commercial PtRu/C and Pd/C catalysts, implying that the anti-CO poisoning ability is enhanced. Combined with the analysis of X-ray diffraction (XRD), high-resolution transmission electron microscopy (HRTEM), X-ray photoelectron spectroscopy (XPS) and Raman, the enhanced catalytic activity and anti-CO poisoning ability are attributed to the charge transfer and lattice compression between Pd and Cu, which modify the d-band center and weaken the adsorption of CO. Furthermore, a volcano plot is found between the MOR activity and d-band center, indicating that the excellent MOR activity is attributed to the optimal d-band center with the moderate adsorption strength of CO-like intermediates.
研究领域:
材料科学
·
电化学
·
催化反应
✓ 已验证
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2021
·
IF 6.901
Na Ye,Yanxin Bai,Zhao Jiang,Tao Fang
For the first time, PdCu/TaN C catalyst with a special core-shell structure is assembled, which exhibits high catalytic performance for methanol oxidation reaction (MOR) in alkaline medium (1326.95 A g Pd −1 ) and formic acid oxidation reaction (FAOR) in acidic medium (1052.63 A g Pd −1 ), 6.3 and 4.9 times those of the commercial Pd/C, respectively. According to the results of Tafel, Electrochemical Impedance Spectroscopy (EIS), CO stripping and chronoamperometry (CA), it is revealed that the reaction kinetics, anti-CO poisoning ability and stability of PdCu/TaN C for MOR and FAOR are all enhanced significantly. Density Functional Theory (DFT) calculations also indicate that the adsorption intensity of CO is weakened and the binding intensity of OH is enhanced on the Pd 3 Cu 1 /TaN(001) surface, which are beneficial to the removal of adsorbed CO and enhancement of the anti-CO poisoning ability. Combined with the characterization analysis and theoretical calculations, the good catalytic performance of PdCu/TaN C for MOR and FAOR can be attributed to the unique electronic structure and morphology from the effective interface, geometric effects and proper d-band center.
研究领域:
电化学
·
催化材料
·
理论计算
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）