CHINESE JOURNAL OF CATALYSIS
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2018
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IF 3.525
Di Zhang,Jingjie Luo,Jiajie Wang,Xin Xiao,Yuefeng Liu,Wei Qi,Dang Sheng Su,Wei Chu
A series of Ru/FeO x catalysts were synthesized for the selective hydrogenation of CO 2 to CO. Detailed characterizations of the catalysts through X-ray diffraction, X-ray photoelectron spectroscopy, transmission electron microscopy, and temperature-programmed techniques were performed to directly monitor the surface chemical properties and the catalytic performance to elucidate the reaction mechanism. Highly dispersed Ru species were observed on the surface of FeO x regardless of the initial Ru loading. Varying the Ru loading resulted in changes to the Ru coverage over the FeO x surface, which had a significant impact on the interaction between Ru and adsorbed H, and concomitantly, the H 2 activation capacity via the ability for H 2 dissociation. FeO x having 0.01% of Ru loading exhibited 100% selectivity toward CO resulting from the very strong interaction between Ru and adsorbed H, which limits the desorption of the activated H species and hinders over-reduction of CO to CH 4 . Further increasing the Ru loading of the catalysts to above 0.01% resulted in the adsorbed H to be easily dissociated, as a result of a weaker interaction with Ru, which allowed excessive CO reduction to produce CH 4 . Understanding how to selectively design the catalyst by tuning the initial loading of the active phase has broader implications on the design of supported metal catalysts toward preparing liquid fuels from CO 2 .
研究领域:
催化化学
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材料科学
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DOI
高影响因子
Science China-Chemistry
·
2022
·Vol. 65
·期 3
·521-531
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IF 10.138
Chen Zhida,Chen Wenda,Zheng Lirong,Huang Tao,Hu Jing,Lei Yaqi,Yuan Qi,Ren Xiangzhong,Li Yongliang,Zhang Lei,Huang Shaoluan,Ye Shenghua,Zhang Qianling,Ouyang Xiaoping,Sun Xueliang,Liu Jianhong
In this study, the morphological distribution of Ru on nitrogen-doped graphene (NG) could be rationally regulated via modulating the combination mode between Ru precursor and the zeolite imidazolate framework-8 (ZIF-8). The cation exchange and host-guest strategies respectively resulted in two different combination modes between Ru precursor and ZIF-8 anchored on graphene. Following pyrolysis of the above precursors, Ru single-atom sites (SASs) with and without Ru nanoparticles (NPs) were formed selectively on NG (denoted as Ru SASs+NPs/NG and Ru SASs/NG, respectively). Ru SASs+NPs/NG exhibited excellent hydrogen evolution reaction (HER) performance in alkaline solutions ( η 10 =12 mV, 12.57 A mg −1 Ru at 100 mV), which is much better than Ru SASs/NG. The experimental and theoretical study revealed that Ru SASs could adsorb hydrogen with optimal adsorption strength, while Ru NPs could lower the barrier of water molecule dissociation, and thus Ru SASs and Ru NPs could synergistically promote the catalytic performance of HER in alkaline solutions.
研究领域:
材料科学
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催化化学
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Lingxin Peng,Liang Su,Xu Yu,Rongyan Wang,Xiangzhi Cui,Han Tian,Shaowen Cao,Bao Yu Xia,Jianlin Shi
Developing efficient electrocatalysts is of significance for hydrogen production in acid electrolyte. In this work, we report a facile decoration of ruthenium species onto tungsten oxides to construct the Mott-Schottky heterojunction electrocatalyst for hydrogen evolution. The resultant Ru-WO 2.72 hybrid exhibits a superior Ru-based mass activity of 161.6 times higher than that of commercial Ru/C for hydrogen evolution, featuring a Tafel slope of 50 mV dec −1 and 40 mV overpotential at the current density of 10 mA cm −2 . The uniform distribution of Ru species triggers a strong electron transfer across the Ru-WO 2.72 Schottky barrier, resulting in a largely increased local electron density on the active Ru surface. Such electron enrichment induced by the Mott-Schottky effect at the metal-metal oxides interface is responsible for enhanced hydrogen production. This work demonstrates an effective strategy by Mott-Schottky effect to regulate electron distribution, which would evoke more inspiration in designing efficient electrocatalysis and beyond.
研究领域:
电化学
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催化材料科学
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DOI
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
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2024
·Vol. 30
·期 37
·e202400945
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IF 3.9
Zhiqian Lin,Haoxian Zhu,Liyuan Qian,Xiaohui Tang,Jiangnan Wen,Yun Wang,Xiaofei Wang,Songbai Han,Jinlong Zhu,Haibin Lin,Yusheng Zhao
Graphical The well-dispersed Ru in the Co−NC carbon matrix altered the total charge distribution over the Co−N−C catalytic sites and led to the formation of electron-rich Co−N, which is highly active for the polysulfide conversion reactions. Additionally, introducing Ru in the Co−NC matrix provided additional catalytic sites over the Ru−N x species to manifest optimal adsorption behavior of polysulfides. The performance of lithium-sulfur batteries is compromised by the loss of sulfur as dissolved polysulfides in the electrolyte and consequently the polysulfide redox shutting effect. Accelerating the conversion kinetics of polysulfide intermediates into sulfur or lithium sulfide through electrocatalysis has emerged as a root-cause solution. Co−N−C composite electrocatalyst is commonly used for this purpose. It is illustrated here that how the effectiveness can be improved by modulating the coordination chemistry of Co−N−C catalytic sites through introducing Ru species (RuCo−NC). The well-dispersed Ru in the Co−NC carbon matrix altered the total charge distribution over the Co−N−C catalytic sites and led to the formation of electron-rich Co−N, which is highly active for the polysulfide conversion reactions. Using Ru to modulate the electronic structure in the Co−N−C configuration and the additional catalytic sites over the Ru−N x species can manifest optimal adsorption behavior of polysulfides. Consequently, the sulfur cathode with RuCo−NC can reduce the capacity fade rate from 0.11 % per cycle without catalyst (initial capacity of 701 mAh g −1 ) to 0.054 % per cycle (initial capacity of 1074 mAh g −1 ) over 400 cycles at 0.2 C rate. The results of this study provide the evidence for a feasible catalyst modification strategy for the polysulfide electrocatalysis.
研究领域:
材料科学
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电化学
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产品关联
DOI
PubMed
高影响因子
ChemCatChem
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2021
·Vol. 13
·期 19
·4159-4163
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IF 5.686
Dongxia Jiao,Yehong Wang,Zhixin Zhang,Jian Zhang,Lijun Lei,Feng Wang
Graphical Synthetic methods : We designed a hydroxyapatite (HAP)-stabilized, positively charged Ru-based catalyst which can efficiently catalyze the formylation reaction of amines with CO for the synthesis of formamide. The combination of characterization results and control experiments showed that positively charged Ru species, particularly the hydrated RuO x particles on the surface were essential to the high catalytic activity of Ru-HAP in the formylation reaction. Formamide is an important solvent and synthetic intermediate. Herein, we designed a hydroxyapatite (HAP)-stabilized, positively charged Ru-based catalysts which can efficiently catalyze the formylation reaction of amines with CO for the synthesis of formamide. The Ru-HAP showed excellent catalytic performance in N,N-Dimethylformamide (DMF) synthesis, with about 75 % dimethylamine conversion and >99 % DMF selectivity at 300 h of continuous reaction. The combination of characterization results and control experiments showed that positively charged Ru species, including hydrated RuO x and Ru 3+ species, were catalytically active. In particular, the surface RuO x species were more active than the Ru 3+ species located within the HAP framework.
研究领域:
催化
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材料科学
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化学工程
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无机化学
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DOI
高影响因子
CATALYSIS LETTERS
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2018
·Vol. 149
·期 1
·180-189
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IF 2.911
Hu Yin,Chen Wei,Ba Mingwei,Song Weiguo
Solvent-free selective hydrogenation of α -pinene to synthesize cis -pinane with high efficiency has always been a challenge in the catalytic research. The key to achieve this goal is the development of the highly efficient and recyclable catalysts. Cubic NaNbO 3 crystals were functionalized by (γ-aminopropyl)-triethoxysilane (APTS) and decorated with Ru species by a simple solvothermal approach combined with a sol-gel method. And this compound was applied to the catalytic hydrogenation of α -pinene. The crystal phase, chemical structure and surface components of the catalysts were analyzed by X-ray diffraction, field emission transmission electron microscope, X-ray photoelectron spectroscopy, Fourier transform infrared spectra and thermogravimetric analysis. APTS-functionalization of the catalyst surface contributes to the highly dispersed and uniform Ru species with small particle size, leading to the outstanding conversion of α -pinene and selectivity of cis -pinane over NaNbO 3 /APTS/Ru catalyst. The performance of this catalyst is better than that of other similar catalysts, and is comparable to that of commercial Ru/C. The possible mechanisms of the formation of catalyst and the hydrogenation reaction were proposed and discussed. The decrease of catalytic performance after seven cycles should be ascribed to the decomposition and leaching of APTS during the hydrogenation process. The work provides an alternative strategy to design a kind of reusable catalyst with highly efficient hydrogenation performance based on the surface functionalization. Graphical Abstract
研究领域:
催化
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材料科学
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化学工程
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物理化学
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DOI
高影响因子
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