JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Jinping Wei,Fengxia Wu,Hongda Sun,Shiyu Xia,Xueqing Sang,Fenghua Li,Zhichao Zhang,Shuang Han,Wenxin Niu
Incorporation of oxophilic metals into Pd-based nanostructures has shown great potential in small molecule electrooxidation owing to their superior anti-poisoning capability. However, engineering the electronic structure of oxophilic dopants in Pd-based catalysts remains challenging and their impact on electrooxidation reactions is rarely demonstrated. Herein, we have developed a method for synthesizing PdSb-based nanosheets , enabling the incorporation of the Sb element in a predominantly metallic state despite its high oxophilic nature. Moreover, the Pd 90 Sb 7 W 3 nanosheet serves as an efficient electrocatalyst for the formic acid oxidation reaction (FAOR), and the underlying promotion mechanism is investigated. Among the as-prepared PdSb-based nanosheets, the Pd 90 Sb 7 W 3 nanosheet exhibits a remarkable 69.03% metallic state of Sb, surpassing the values observed for the Pd 86 Sb 12 W 2 (33.01%) and Pd 83 Sb 14 W 3 (25.41%) nanosheets. X-ray photoelectron spectroscopy (XPS) and CO stripping experiments confirm that the Sb metallic state contributes the synergistic effect of their electronic and oxophilic effect, thus leading to an effective electrooxidation removal of CO and significantly enhanced FAOR electrocatalytic activity (1.47 A mg −1 ; 2.32 mA cm −1 ) compared with the oxidated state of Sb. This work highlights the importance of modulating the chemical valence state of oxophilic metals to enhance electrocatalytic performance, offering valuable insights for the design of high-performance electrocatalysts for electrooxidation of small molecules.
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
APPLIED SURFACE SCIENCE
·
2018
·
IF 4.439
Xue Li,Yan-Rong Liu,Wen-Min Liao,Ai-Ping Jia,Yue-Juan Wang,Ji-Qing Lu,Meng-Fei Luo
Catalytic propane combustion was performed on a series of supported Pt/AlF 3 catalysts. These catalysts are very active and stable in the reaction, and the 0.2Pt/AlF 3 catalyst gives the highest specific reaction rate of 207.3 μmol g Pt −1 s −1 at 220 °C. The 1Pt/AlF 3 is much more active than the reference Pt/Al 2 O 3 catalyst, due to its higher content of metallic Pt species than that in the Pt/Al 2 O 3 . Furthermore, turnover frequency (TOF) based on Pt dispersion increases with the surface concentration of metallic Pt 0 in the catalyst, suggesting these species might be the active sites. Furthermore, synergistic roles of metallic and oxidized Pt species are found, as the TOFs calculated based on surface Pt 0 concentration reaches a maximum at the Pt 0 /Pt 2+ molar ratio of about 1. Such optimal Pt 0 /Pt 2+ ratio implies the requirement of Pt 0 Pt 2+ pair in the reaction, probably due to the activation and cleavage of C H bond on metallic Pt atom and the sequential oxidation on the oxidized Pt atoms.
研究领域:
催化化学
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环境化学
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材料化学
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表面科学
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能源化学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Weihao Bai,Hao Li,Gang Peng,Jinnan Wang,Aimin Li,Philippe François-Xavier Corvini
Although ferrocene (Fc) based Metal-Organic Frameworks (MOFs) can act as oxygen evolution co-catalysts (OECs) for improvement of catalytic reactivity, the poor conductivity and lack of highly active metal sites limit its further application in photoelectrochemical (PEC) water splitting. Herein, the amorphous NiFc-MOF was grafted on BiVO 4 photoanode (BiVO 4 @ a NiFc-MOFs) for efficient PEC water splitting. This novel BiVO 4 @ a NiFc-MOFs exhibits high current density of 4.34 mA cm −2 at 1.23 V RHE and relative low onset potential of 0.223 V RHE . The subsequent characterizations demonstrate that Ni species with metal-like state in bulk of a NiFc-MOFs form strong metal-support interaction with BiVO 4 , thereby promoting the interfacial charge transfer. Moreover, the surface of a NiFc-MOFs is short-range ordered with abundant coordinatively unsaturated Ni sites, creating a more favorable pathway for oxygen evolution reaction from thermodynamics. This work provides a simple method to design photoanodes with efficient OECs of amorphous MOFs for feasible PEC water splitting application.
研究领域:
材料科学
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光化学
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电化学
·
催化
✓ 已验证
产品关联
DOI
高影响因子
Advanced Energy Materials
·
2022
·Vol. 12
·期 37
·2201734
·
IF 29.698
Qi Li,Jun Zhang,Lixiang Zhong,Fushan Geng,Ying Tao,Chuannan Geng,Shuzhou Li,Bingwen Hu,Quan-Hong Yang
Hard carbons have been identified as competitive anodes for Li/Na/K-ion batteries but their Li/Na/K-ion storage mechanisms significantly vary in different batteries. It is fundamental to understand the basic science behind the difference. Herein, it is theoretically revealed that defects on the carbon layers generally have an influential impact on the atomic interactions including the metal–metal (M–M) and metal–carbon (M–C) interactions, thereby determining whether the stored alkali-metal atoms are in ionic or quasi-metallic states. Upon increasing the number of metal atoms on a carbon layer composed of only hexatomic rings, K tends to be stored in an ionic state similar to Li due to the dominant M–C interaction, while on a carbon layer with defects, K tends to be stored in a quasi-metallic state similar to Na due to the dominant M–M interaction. For experimental verification, a glassy carbon, the extreme form of hard carbon with dominant sp 2 hybridization and only Stone–Wales defects, is selected as a model anode, and its Li/Na/K-ion storage mechanisms are exactly consistent with the theoretical prediction. More profoundly, for the first time, the quasi-metallic K cluster information is captured by ex situ electron paramagnetic resonance.
研究领域:
材料科学
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电化学
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电池技术
✓ 已验证
产品关联
DOI
高影响因子
Catalysts
·
2025
·Vol. 15
·期 7
·694
·
IF 4
Ziyan Mi,Huayun Long,Yuhua Jia,Yue Ma,Cuilan Miao,Yan Xie,Xiaomei Zhu,Jiahui Huang
The development of non-noble metal catalysts for gas-phase propylene epoxidation with H2/O2remains challenging due to their inadequate activity and stability. Herein, we report a Cs+-modified Ni/TS-1 catalyst (9%Ni-Cs/TS-1), which exhibits unprecedented catalytic performance, giving a state-of-the-art PO formation rate of 382.9 gPO·kgcat−1·h−1with 87.8% selectivity at 200 °C. The catalyst stability was sustainable for 150 h, far surpassing reported Ni-based catalysts. Ni/TS-1 exhibited low catalytic activity. However, the Cs modification significantly enhanced the performance of Ni/TS-1. Furthermore, the intrinsic reason for the enhanced performance was elucidated by multiple techniques such as XPS, N2physisorption, TEM,29Si NMR, NH3-TPD-MS, UV–vis, and so on. The findings indicated that the incorporation of Cs+markedly boosted the reduction of Ni, enhanced Ni0formation, strengthened Ni-Ti interactions, reduced acid sites to inhibit PO isomerization, improved the dispersion of Ni nanoparticles, reduced particle size, and improved the hydrophobicity of Ni/TS-1 to facilitate propylene adsorption/PO desorption. The 9%Ni-Cs/TS-1 catalyst demonstrated exceptional performance characterized by a low cost, high activity, and long-term stability, offering a viable alternative to Au-based systems.
研究领域:
催化化学
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化学工程
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材料科学
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多相催化
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绿色化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）