ACS Catalysis
·
2022
·
IF 13.7
Min Huang,Shuyi Zhang,Bo Wu,Yao Wei,Xing Yu,Yongping Gan,Tiejun Lin,Fei Yu,Fanfei Sun,Zheng Jiang,Liangshu Zhong
Direct selective methane photooxidation to liquid oxygenates with high productivity and selectivity under mild reaction conditions is highly urgent but remains challenging. Herein, a Cu and W codoped TiO2 (Cu–W–TiO2) photocatalyst was fabricated to enable aerobic oxidation of methane into oxygenates with limited formation of CO2 under ambient temperature. A high oxygenate productivity of 34.5 mmol g–1 with a remarkable selectivity of 97.1% was achieved over the Cu–W–TiO2 photocatalyst. Based on structural characterizations and mechanism studies, it was suggested that the Cu species acted as hole traps, while oxygen vacancies and the W6+-dopant state worked as electron traps. The inhibited recombination of photogenerated carriers contributed to enhanced photocatalytic efficiency. The modulated electronic and band structure promoted the activation of methane and hindered the overoxidation of oxygenates.
研究领域:
化学
·
材料科学
·
环境科学
·
催化
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DOI
高影响因子
Small
·
2026
·
IF 11.8
Hui Wang,Xiang Li,Zitong Jiang,Qing Xu,Qiaoqin Guo,Chaozheng He,Junjun Zhang,Yaming Liu,Mingshang Jin
Direct ethanol fuel cells are promising clean energy devices, but the difficulty in cleaving the C─C bond of ethanol leads to low C1 pathway selectivity (typically ∼10%) and incomplete energy conversion. To address this challenge, we synthesized a porous multiphase Pd-based metallene nanocatalyst co-doped with oxygen-philic Cu and W. Temperature was identified as the key factor regulating the crystal structure: low temperatures yielded amorphous phases, high temperatures produced crystalline phases, and intermediate temperatures formed the desired crystalline/amorphous mixed multiphase structure. This multiphase structure provided abundant active sites. The optimal PdCuW metallene exhibited exceptional performance for ethanol electrooxidation: a record-high C1 pathway selectivity of 72.6% (1.6 times that of undoped Pd metallene and 10.2 times that of commercial Pd/C), a mass activity of 4301.6 mA/mg Pd (4.7 times that of commercial Pd/C), and superior stability (only 7.3% activity decay vs. 67.9% for commercial Pd/C). Mechanistic studies (In situ ATR-FTIR, DFT calculations) revealed that synergistic Cu-W doping reduced the C─C bond cleavage energy barrier, enhanced OH * adsorption, and weakened the poisoning effect of intermediate CO * . The work offers a rational design strategy for high-selectivity electrocatalysts, advancing ethanol's full energy utilization and holding broad implications for Pd-based catalyst systems in energy conversion technologies.
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DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 6
·124949
·
IF 7.5
Jiamin Wang,Tengjuan Ma,Yulong Ma,Jinpeng Wei,Haiyan Yan,Yonggang Sun
In recent years, developing highly active non-noble metal catalysts for biomass hydrodeoxygenation (HDO) to achieve value-added conversion has attracted significant attention. However, major challenges remain in catalyst efficiency, stability, and the precise control of reaction pathways.In this study, a synergistic Ni-W-Cu mixed metal oxide (MMO) catalyst was prepared from LDH precursors via a stepwise "ion exchange-active site introduction" strategy. Under optimized conditions (240 ℃, 2.5 MPa H 2 , 2.5 h), the catalyst achieved complete cellulose conversion with 72% ethylene glycol selectivity. Even after five reuse cycles, it retained 95.4% conversion and 62% selectivity. Characterization demonstrated that appropriate Cu loading promoted Ni-Cu alloying and modulated Ni electronic structure, which induced abundant W 6 + /W 4+ species and oxygen vacancies (O V ). In this architecture, W 6+ provides Lewis acidity, while W 4+ couples tightly with O V , thereby synergistically enhancing the catalyst's hydrogenation capability and bond-cleavage ability. Density functional theory (DFT) calculations reveal that the strong interaction between W and Cu constructs highly efficient adsorption sites, enabling the precise catalysis of C-O bond scission. These findings suggest that tailoring the W-Cu interplay offers a viable strategy for directing product selectivity. By engineering a stable, multifunctional catalyst for biomass conversion, this study provides a new strategy for constructing high-performance HDO catalysts.
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高影响因子
ACTA PHYSICO-CHIMICA SINICA
·
2017
·Vol. 33
·期 5
·993-1000
·
IF 0.767
YANG Kun,YAO Qi-Lu,LU Zhang-Hui,KANG Zhi-Bing,CHEN Xiang-Shu
Noble-metal-free CuMo nanoparticles (NPs) without surfactant or support have been facilely prepared using NaBH4 as a reducing agent. The as-prepared CuMo nanocatalysts were characterized using X-ray diffraction (XRD), transmission electron microscopy (TEM), high resolution
transmission electron microscopy (HRTEM), selected area electron diffraction (SAED), inductively coupled plasma-atomic emission spectroscopy (ICP-AES), X-ray photoelectron spectroscopy (XPS), and Brunauer-Emmett-Teller (BET) surface area measurements, and used as catalysts for the hydrolysis
of ammonia borane (AB, NH3BH3) at room temperature. The as-synthesized Cu0.9Mo0.1 NPs exhibited a high activity towards the hydrolysis of AB with a turnover frequency (TOF) of 14.9 min-1, a higher value than that reported for Cu catalysts.
Our synthesis is not limited to CuMo NPs alone, but can easily be extended to CuW (3.6 min-1), CuCr (2 min-1), NiMo (55.6 min-1), and CoMo (21.7 min-1) NPs, providing a general approach to Cu-M (M = Mo, W, Cr) and TM-Mo (TM = Cu, Ni, Co) NPs as a
series of novel catalysts for the hydrolysis of AB. The enhanced activity of bimetallic NPs may be attributed to the synergistic effects of the Cu-M NPs induced by the strain and ligand effects.
研究领域:
催化
·
材料科学
·
纳米技术
·
化学工程
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产品关联
DOI
高影响因子