JOURNAL OF CATALYSIS
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2022
·
IF 8.047
Xuliang Pang,Hongye Bai,Yifei Huang,Huaiquan Zhao,Guoli Zheng,Weiqiang Fan
The biomass-derived 5-hydroxymethylfurfural (HMF) oxidation holds great significance for the sustainable production of value-added chemicals. However, the construction of active species with efficient oxidative-activity of alcohol/aldehyde still faces a great challenge. In this work, the reconstruction of CuO/Ni MOF successfully implanted CuOOH/NiOOH and deeply clarified their catalytic mechanism for HMF oxidation. It is worth noting that CuOOH/NiOOH exhibited an excellent self-healing ability during HMF oxidation, further realizing the reproducibility and long-term stability of catalyst. Moreover, a two-chamber electrocatalytic system combining HMF oxidation with 4-nitrophenol hydrogenation was established based on the activated CuO/Ni MOF. As a result, the overall reaction achieved a current density of 47.6 mA/cm 2 at 0.55 V vs Ag/AgCl (3.0 h), and the corresponding conversion rate and Faraday efficiency reached nearly 100 %. This study provides new insight into the electrocatalytic-reconstruction strategy to implant active species for alcohol/aldehyde oxidation.
研究领域:
化学
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催化材料科学
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产品关联
DOI
高影响因子
Science Bulletin
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2023
·
IF 18.9
Ye Wang,Ming Xu,Xi Wang,Ruixiang Ge,Yu-Quan Zhu,An-Zhen Li,Hua Zhou,Fengen Chen,Lirong Zheng,Haohong Duan
Electrocatalytic oxidation of renewable biomass (such as glucose) into high-value-added chemicals provides an effective approach to achieving carbon neutrality. CuO-derived materials are among the most promising electrocatalysts for biomass electrooxidation , but the identification of their active sites under electrochemical conditions remains elusive. Herein, we report a potential-dependent structure evolution over CuO in the glucose oxidation reaction (GOR). Through systematic electrochemical and spectroscopic characterizations, we unveil that CuO undergoes Cu 2+ /Cu + and Cu 3+ /Cu 2+ redox processes at increased potentials with successive generation of Cu(OH) 2 and CuOOH as the active phases. In addition, these two structures have distinct activities in the GOR, with Cu(OH) 2 being favorable for aldehyde oxidation, and CuOOH showed faster kinetics in carbon–carbon cleavage and alcohol/aldehyde oxidation. This work deepens our understanding of the dynamic reconstruction of Cu-based catalysts under electrochemical conditions and may guide rational material design for biomass valorization.
研究领域:
电化学
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催化
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材料科学
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可再生能源
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产品关联
DOI
PubMed
高影响因子
ELECTROANALYSIS
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2018
·Vol. 30
·期 6
·1033-1040
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IF 2.851
Bo Li,Yongzhao Fan,Changqing Li,Xu Zhao,Kun Liu,Yuqing Lin
This study for the first time establishes a reliable non-enzymatic online electrochemical system (OECS) for selective and continuous measuring glucose in animal cerebral system. We proposed a one-step electrochemical method to synthetize a Cu nanostructure directly onto electrode, and over-oxidize it in NaOH to form acanthosphere-like CuOOH nanospheres (denoted as AN-CuOOH), which can serve as an excellent electrochemical catalyst for glucose oxidation and thus for simple and reproducible non-enzymatic glucose detection in strong alkaline solution. To validate the AN-CuOOH-based sensors for in vivo applications, we connect the sensors to a merged solution of in vivo microdialysis and 0.4 M NaOH to set up an OECS for in vivo glucose monitoring in rat brain. The response of this system has strong tolerance to the oxygen and pH fluctuation which may happen in the cerebral brain system during some physiological and pathological processes. The fabricated non-enzymatic OECS has a good linear current response to glucose within a concentration range from 10 to 1000 μΜ with sensitivity of 130.22 nA ⋅ μΜ −1 cm −2 . Additionally, the OECS is stable and does not suffer from the interference coexisting in the cerebral system. With the fabricated non-enzymatic OECS for glucose measurement, the basal level of glucose in the microdialysate from rats striatum was determined to be 248.63 μΜ (n=3). Furthermore, the glucose was clearly decreased to 26.37 % of the basal level when the rat was undergone by 20 min ischemia, and the glucose concentration was gradually restored to 99.15 % during 40 min of reperfusion. Our work propose a technically simple strategy for the fabrication of a highly reproducible non-enzymatic OECS system free from oxygen and pH interference, which is promising in exploring the molecular mechanism associated with brain functions.
研究领域:
生物医学工程
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神经科学
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分析化学
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产品关联
DOI
高影响因子
ACS Catalysis
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2022
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IF 13.7
Xuliang Pang,Hongye Bai,Huaiquan Zhao,Weiqiang Fan,Weidong Shi
Electrocatalytic conversion of biomass-derived 5-hydroxymethylfurfural (HMF) to value-added 2,5-furandicarboxylic acid (FDCA) is of great significance for sustainable chemical production. The key challenge is to establish an electrocatalytic system with a wide potential window, which can selectively oxidize HMF to FDCA without causing water oxidation. In this study, Cu foam decorated with Cu(OH)2 (CF-Cu(OH)2) was successfully fabricated as an efficient catalyst, and CuOOH active species generated by electrochemistry were demonstrated as the main catalytic sites for HMF oxidation. As a result, the current density of CF-Cu(OH)2 reached up to 198.2 mA/cm2 (100 mM HMF, 1.0 M KOH, 0.8 V vs Ag/AgCl), and a high faradic efficiency close to 100% for FDCA production (yield: 98.7%) was realized. Moreover, we reveal the mechanism for the electro-oxidation of HMF to FDCA and further provide an insight into the oxidation pathway for HMF. A paired electrochemical system exhibits superior catalytic performance of synergetic reactions (HMF oxidation and 4-NP reduction). Therefore, this work proposes a strategy to simultaneously produce two types of value-added chemicals at both electrodes, which can be applied in other electrocatalytic systems for the green synthesis of organic compounds.
研究领域:
电化学
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催化
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可持续化学
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生物质转化
✓ 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）