APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
·
IF 24.319
Bowen Yuan,Jian Zhang,Zhe An,Yanru Zhu,Xin Shu,Hongyan Song,Xu Xiang,Wanning Wang,Yusheng Jing,Lirong Zheng,Jing He
Transformation of ethanol to more valuable C 4+ alcohols by coupling reaction has been of great interest from the point of view of chemistry and technology of biomass utilization. This work reports atomic Ru on Mg and Al containing layered double oxides (MgAl-LDO) for ethanol coupling to C 4+ alcohols. The atomic Ru remarkably promotes the coupling of ethanol, achieving a selectivity of 82.6% to C 4+ alcohols under an ethanol conversion of 29.6%. Through tailoring Ru dispersion and acid-base properties, it has been found that atomic Ru promotes ethanol dehydrogenation and the following aldol condensation of acetaldehyde.
研究领域:
化学
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催化技术
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生物质利用
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Rong Shang,Qizhao Zhang,Peng Lin,Bang Gu,Qinghu Tang,Qiue Cao,Wenhao Fang
Direct oxidative coupling of alcohols and amines is an environmental-benign and atomic-economy approach for imine synthesis. We disclosed that UiO-66 framework successfully confined Ru to single-atom scale with assistance of oxophilic Zn 2+ promoter. This RuZn@UiO-66 catalyst showed a highest TOF of 78 h -1 among all Ru catalysts in literature and attained > 99% yield to benzylideneaniline in the model reaction in an O 2 atmosphere at a low temperature without alkaline additives. In addition, this catalyst demonstrated satisfying gram-scale imine synthesis, wide substrate scope and stable reusability. Kinetic investigations and in situ characterizations allowed getting insights to active sites, amphoteric carrier and reaction mechanism. Dynamic interactions between Ru and Zn based on their ratios induced electron-deficient Ru 0 active sites promoted by oxophilic Zn 2+ species. Hence, primary alcohols can be efficiently converted to the corresponding aldehydes using molecular O 2 , i.e. , the rate-determining step. Besides, Zr 4+ -O 2- pairs on UiO-66 provided adequate acidic-basic sites for the tandem catalysis.
研究领域:
催化化学
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材料科学
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环境化学
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产品关联
DOI
高影响因子
ADVANCED MATERIALS
·
2025
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IF 26.8
Hang Wang,Han Xu,Fei Yang,Yan Qing,Fuxiang Chu,Yiqiang Wu,Sheng Ye,Fuquan Xiong
Local electric fields of the electrocatalysts can modulate adsorbate binding energies based on their polarizability and dipole moment, which directly influence the catalytic performance. Nevertheless, implementing the prevailing strategy remains challenging due to the scarcity of active sites and sluggish catalytic kinetics. Herein, a continuous heterogeneous-curvature nanoreactor (HeterC-LCS) is created to enhance local electric fields by optimizing the uniform-nanocurvature with tip effects. The H + concentration and H 2 O transmission rate of HeterC-LCS are improved by about 2.1 and 1.7 times that of the homogeneous curvature structure (HomoC-LCS) during the hydrogen evolution reaction (HER) process. Besides, HeterC-LCS demonstrates a rapid kinetics of intermediate transformation and an extremely low energy barrier. Such HeterC-LCS depicts a lowest overpotential of 9.2 mV at 10 mA cm −2 , which outperforms all known carbon- and Ru-based electrocatalysts. And the mass activity is approximately 60 times that of commercial Pt/C. This work proposes a novel strategy of uniform-nanocurvature optimized by tip effects toward industrially electrocatalytic HER.
研究领域:
电催化
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纳米材料科学
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物理化学
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能源化学
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表面科学
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材料化学
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电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHINESE JOURNAL OF CATALYSIS
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2023
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IF 16.5
Ce Han,Bingbao Mei,Qinghua Zhang,Huimin Zhang,Pengfei Yao,Ping Song,Xue Gong,Peixin Cui,Zheng Jiang,Lin Gu,Weilin Xu
Regulation of the atomic distribution is crucial for the development of atomically dispersed electrocatalysts. In this study, atomic Ru coordinated by channel ammonia in V-doped tungsten bronze (Ru/V-NHWO, Ru 0.44 wt%, V 0.45 wt%) was used as a high-performance catalyst for the hydrogen evolution reaction (HER), demonstrating remarkable mass activity in a wide pH range. Atomic Ru with a regulated spatial distribution and electronic structure was achieved owing to its unique coordination with the ammonia species in the hexagonal channels of V-NHWO. V doping in NHWO led to enhanced intrinsic activity and conductivity. Theoretical calculations revealed that the multichannel, vertically integrated Ru sites in the V-doped channels, as well as the coexisting Ru sites without multichannels or V-doping, improved the free energy of water dissociation and hydrogen sorption , which boosted the HER activity. Our study paves a new way for constructing atomically dispersed materials with a regulated spatial distribution for diverse applications.
研究领域:
材料科学
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电化学
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催化
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能源材料
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产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2019
·Vol. 7
·期 33
·19531-19538
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IF 10.733
Qi Hu,Guomin Li,Xiaowan Huang,Ziyu Wang,Hengpan Yang,Qianling Zhang,Jianhong Liu,Chuanxin He
Regulation of the electronic structures of metal centers represents a robust strategy for enhancing the activity of electrocatalysts. Herein, we report the crafting of hybrid electrocatalysts comprising both single atomic Ru (SA-Ru) and Ru nanoparticles (NPs) supported on porous N-doped carbon (PC), in which the electronic structures of SA-Ru were effectively optimized by nearby Ru NPs to achieve great enhancement of the hydrogen evolution reaction (HER). The resulting SA-Ru/Ru NPs/PC displayed ultrahigh activity for HER in 1 M KOH with a mass activity of 4.2 mA μgRu−1 at −0.07 V vs. RHE; this activity was 14 times that of commercial Pt/C, representing the largest reported value among the Pt-free electrocatalysts. In addition to the ultrahigh activity, the composite possessed the outstanding stability of 24 h and rapid HER kinetics (i.e. Tafel slope: 31.8 mV dec−1). The experimental and theoretical results matched well with each other and unambiguously indicated that the control over the electronic structures of SA-Ru and the advantageous PC support (i.e. its hierarchical porous nanostructures and superhydrophilic surface) jointly contributed to the exceptional performance.
研究领域:
材料科学
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电化学
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催化
✓ 已验证
产品关联
DOI
高影响因子
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