Small
·
2024
·Vol. 20
·期 52
·2408373
·
IF 13
Xiaotong Zhou,Songliang Liu,Huaifang Teng,Kun Ma,Weixin Miao,Xuejing Cui,Xin Zhou,Luhua Jiang
Reasonable construction of high activity and selectivity electrocatalysts is crucial to achieve efficient ethanol oxidation reaction (EOR). However, the oxidation of ethanol tends to produce CO species that poison the active centers of the EOR electrocatalysts. Herein, a unique amorphous CrO x -protected defect-rich ultrafine Pd nanowires (CrO x -Pd NWs) is developed. On the one hand, the CrO x layer can act as a protective layer to maintain the structure of the nanowire. On the other hand, it can play the role of OH regulator to optimize the adsorption energy barrier of intermediate species in Pd nanowire, thereby enhancing the ability of the catalyst to resist CO poisoning. The CrO x -Pd NWs exhibit excellent EOR performance with 3.64 times higher mass activity and 50 mV lower CO electro-oxidation potential than commercial Pd black. The results show that the CrO x layer promotes the dissociation of H 2 O into OH ads , while the CrO x transfers electrons to neighboring Pd atoms optimizing the electronic configuration of Pd, thus selectively oxidizing ethanol to acetate and preventing the formation of toxic * CO. This work provides an effective strategy for the synthesis of nanowire materials with oxide/metal interfaces and offers new ideas for the design of catalysts that can efficiently drive EOR.
研究领域:
材料科学
·
电催化
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Jialu Huang,Chengwei Deng,Yue Liu,Tingting Han,Feng Ji,Yuehua Zhang,Hongbin Lu,Ping Hua,Bowei Zhang,Tao Qian,Xiaolei Yuan,Yaoyue Yang,Yong Yao
Palladium (Pd) is supposed to be one of the most promising catalytic metals towards ethanol (C 2 H 5 OH) oxidation reaction (EOR). However, Pd electrocatalysts easily suffer from the poisoning of the intermediates (especially CO), resulting in the quick decay of EOR catalysis. Herein, inspired by the Brønsted-Lowry acid-base theory, a “attraction–repulsion” concept is proposed to guide the surface structure engineering toward EOR catalysts. Specifically, we induce Bi(OH) 3 species as Brønsted base onto PdBi nanoplates to effectively repel the adsorption of CO intermediates. The PdBi-Bi(OH) 3 nanoplates show an impressive mass activity of 4.46 A mg Pd -1 during the EOR catalysis and keep excellent stability. Both the stability and enhanced performance are attributed by the interfacial Brønsted base Bi(OH) 3 which can selectively attract and repel reactants and intermediates, as evidenced from in situ measurements and theoretical views.
研究领域:
材料科学
·
电化学
·
催化作用
✓ 已验证
产品关联
DOI
PubMed
高影响因子
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
Nanoscale
·
2017
·Vol. 9
·期 17
·5467-5474
·
IF 7.367
Yue Sun,Yunjie Zhou,Cheng Zhu,Lulu Hu,Mumei Han,Aoqi Wang,Hui Huang,Yang Liu,Zhenhui Kang
Highly efficient electrocatalysts remain huge challenges in direct methanol fuel cells (DMFCs). Here, a Pt–Co3O4–CDs/C composite was fabricated as an anode electrocatalyst with low Pt content (12 wt%) by using carbon dots (CDs) and Co3O4 nanoparticles as building blocks. The Pt–Co3O4–CDs/C composite catalyst shows a significantly enhanced electrocatalytic activity (1393.3 mA mg−1 Pt), durability (over 4000 s) and CO-poisoning tolerance. The superior catalytic activity should be attributed to the synergistic effect of CDs, Pt and Co3O4. Furthermore, the Pt–Co3O4–CDs/C catalyst was integrated into a single cell, which exhibits a maximum power density of 45.6 mW cm−2, 1.7 times the cell based on the commercial 20 wt% Pt/C catalyst.
研究领域:
材料科学
·
电化学
✓ 已验证
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
Molecular Catalysis
·
2024
·
IF 3.9
Kaili Wang,Tingting Zhou,Jia He,Zhen Cao,Zaiyong Jiang
Pt based electrocatalysts are considered as very promising for methanol oxidation reaction (MOR). Especially, the PtRu alloy catalysts has attracted more and more attentions. However, the catalytic efficiency of PtRu electrocatalyst is seriously hampered originated from the poisoning effect of CO* intermediate during MOR process. Herein, we have regulated the Pt/Ru atom ratio and controlled the morphology to optimize electronic structures of the alloy for achieving excellent MOR performance. The obtained Pt 2 Ru 1 alloy nanowires display the most negative peak potential of CO oxidation in contrast to commercial Pt/C, PtRu/C catalysts, Pt 3 Ru 1 and Pt 1 Ru 1 alloy nanowires, indicating an excellent anti CO poisoning activity. In addition, the adsorption capacity of OH* on Pt 2 Ru 1 alloy nanowires is obviously improved compared to commercial Pt/C and PtRu/C electrocatalysts, which is in favor of the oxidizing of CO* intermediate. Therefore, the Pt 2 Ru 1 alloy nanowires exhibit significantly enhanced specific activity (2.30 mA cm −2 ) and mass activity (1.29 A mg Pt −1 ) towards MOR compared to those of commercial Pt/C and PtRu/C electrocatalysts. The research offers a potential insight for designing highly efficient electrocatalysts for MOR.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2022
·Vol. 12
·期 27
·17012-17019
·
IF 4.036
Yubing Xue,Dashu Pan,Feng Zuo,Songtao Xiao,Xiang Li,Fuyan Lou,Mingming Li,Yinggen Ouyang
A novel self-reactivated catalyst Pt–ThO2/C was prepared for the first time by selecting radioactive material ThO2 as the catalytic additive to address the low activity and toxicity of the anode Pt/C catalyst in a direct ethanol fuel cell. The catalytic activity and resistance to CO poisoning of Pt-6.67 wt%ThO2/C were found to be superior to those of Pt/C–NaBH4 in electrochemical workstation and single-cell tests. It is speculated that the exist of ThO2 not only improves the catalytic activity via the synergistic effect of Pt and Th, but also produces a large amount of radiolysis products, OH radicals, due to 232Th which oxidatively desorbs CO from Pt–COads and solves the CO poisoning problem.
研究领域:
材料科学
·
能源化学
·
放射化学
✓ 已验证
产品关联
DOI
PubMed
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
APPLIED SURFACE SCIENCE
·
2020
·
IF 6.182
Mengran Lou,Ruiying Wang,Lili Yang,Dianzeng Jia,Zhipeng Sun,Luxiang Wang,Yong Guo,Xingchao Wang,Jie Zhang,Hongli Shi
Direct formic acid fuel cells have great application potential in the energy field, but their commercialization is hindered by the CO poisoning and low performance of Pd-based anode catalysts. In this study, novel composite catalysts composed of Pd, organic-inorganic hybrid imidazole ionic liquid polyoxometalates, and N,P-codoped coal-based carbon fibers with good dispersion and smaller Pd nanoparticles were synthesized successfully. Physical and electrochemical characterizations revealed that the as-prepared Pd-based composite catalysts have excellent CO poisoning resistance and enhanced electrocatalytic activity in formic acid electrooxidation. Notably, the CO oxidation onset potential of a catalyst modified by imidazole ionic liquid polyoxometalate with long alkyl chain was 0.1 V lower than that of the unmodified catalyst. The mass activity of the as-prepared Pd catalyst in formic acid oxidation was 754.1 mA mg −1 Pd . It is expected that organic-inorganic hybrid polyoxometalates can be further applied to fuel cell catalysts.
研究领域:
材料科学
·
电化学
·
能源技术
✓ 已验证
产品关联
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
Nano-Micro Letters
·
2025
·Vol. 17
·期 1
·1-14
·
IF 36.3
Liao Yujia,Chen Wen,Ding Yutian,Xie Lei,Yang Qi,Wu Qilong,Liu Xianglong,Zhu Jinliang,Feng Renfei,Fu Xian-Zhu,Luo Shuiping,Luo Jing-Li
A unique catalyst surface where ultrathin Pt edges are modified by the isolated Pd atoms and BiO x adatoms is rational designed and achieved.
The Pd 1 /Pt-BiO x electrocatalyst exhibits an ultrahigh mass activity of 16.01 A mg −1 Pt+Pd toward ethanol oxidation and enables a direct ethanol fuel cell of peak power density of 56.7 mW cm −2 .
The surrounding BiO x adatoms are critical for mitigating CO-poisoning on Pt surface, and the Pd 1 /Pt single-atom alloy further facilitates the electrooxidation of CH 3 CH 2 OH.
研究领域:
材料科学
·
电化学
✓ 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）