CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Sensen Zhou,Yueli Wen,Bin Wang,Maohong Fan,Lu Ren,Zheng Cui,Wei Huang,Jing Li,Jianping Guo
CO 2 hydrogenation to C 2+ OH is an effective way to diminish CO 2 emissions. Although challenges still exist in large-scale applications, CuFeZn catalysts attract extensive attention due to their low-cost. Herein, CuFeZn catalysts are modified by different amounts of K 3 PO 4 , (KP) 0.1 CuFeZn exhibits an excellent catalytic performance (total alcohols selectivity of 15.76 % at CO 2 conversion of 38.10 %, C 2+ OH/ROH fraction of 94.23 %, and C 2+ alcohols space–time-yield (STY) of 53.81 mg·mL −1 ·h −1 ). Combined with a series of characterization results, it is found that the effect of K 3 PO 4 is complex, and the proportion of Fe 2+ , Cu 0 and medium base shows perfect linear relation to STY of C 2+ OH. The significance level of the above three factors is in the following sequence: Cu 0 ＞Fe 2+ ＞medium base. The introduction of K 3 PO 4 decreases the proportion of Fe 2+ (active site for RWGS, the competitive reaction for C–C coupling) and increases the proportion of Cu + /(Cu + +Cu 0 ) (Cu + is the active site for C–C coupling) due to the synergistic effect of Cu 0 and Cu + , thereby improving the synthesis of C 2+ OH. Moreover, conversion of Fe 0 to Fe 3 C or Fe 3 O 4 plays negative roles in the stability of the catalysts.
研究领域:
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
ChemistryOpen
·
2021
·Vol. 10
·期 5
·560-566
·
IF 2.911
Yingshuang Hui,Yulu Zhan,Wenrong Hou,Lou Gao,Yahong Zhang,Yi Tang
Graphical The product control of C6 aldose toward C6, C4 and C2 alditols have been achieved, which have depended on the well-matched between retro-aldol condensation and hydrogenation process driving by temperature, H 2 pressure and injection modes. Alcohols have a wide range of applicability, and their functions vary with the carbon numbers. C6 and C4 alditols are alternative of sweetener, as well as significant pharmaceutical and chemical intermediates, which are mainly obtained through the fermentation of microorganism currently. Similarly, as a bulk chemical, C2 alditol plays a decisive role in chemical synthesis. However, among them, few works have been focused on the chemical production of C4 alditol yet due to its difficult accumulation. In this paper, under a static and semi-flowing procedure, we have achieved the product control during the conversion of C6 aldose toward C6 alditol, C4 alditol and C2 alditol, respectively. About C4 alditol yield of 20 % and C4 plus C6 alditols yield of 60 % are acquired in the one-pot conversion via a cascade retro-aldol condensation and hydrogenation process. Furthermore, in the semi-flowing condition, the yield of ethylene glycol is up to 73 % thanks to its low instantaneous concentration.
研究领域:
生物化学
·
有机化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF CATALYSIS
·
2024
·
IF 6.5
Wei Jia,Wengang Liu,Yuandong Cui,Hang Song,Chengfeng Zhou,Wei Jiang,Haoxi Ben,Xiaoli Yang,De Chen
Converting cellulose into C 2 alcohols presents a sustainable alternative to fossil fuels, contributing to the development of eco-friendly and economically viable biofuels and chemicals. Tungsten oxide (WO 3 ) is a key solid acid catalyst for this process, yet limited research explores its diverse morphologies and unique catalytic effects. This study investigates diverse WO 3 morphologies (nanosheets, nanoflowers, nanoblocks, and tetrahedral octahedra) in combination with Pd for converting cellulose to C 2 alcohols. Optimized conditions with Pd/o-WO 3 catalyst resulted in the highest C 2 alcohols (ethylene glycol and ethanol, 80.9 %), notably yielding 64.8 % ethylene glycol. Extensive characterizations and DFT calculations reveal the smaller element occupancy rates and a longer W-O bond length led to a large number of crystal defects over Pd/o-WO 3 . It facilitated the formation of W 5+ –OH sites and Pd-O(H)-W interactions, further synergistically enhancing hydrogenation ability and acidity. Designed experiments to elucidate cellulose conversion pathways, including hydrolysis, retro -aldol condensation, and hydrogenation. This study emphasizes the unique impact of WO 3 morphologies and underscores the importance of supporting crystal defects for catalytic performance in eco-friendly biofuel and chemical production.
研究领域:
催化化学
·
可再生资源与环境科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Wei Jia,Hang Song,Dandan Wang,Chengfeng Zhou,Yuling Zhao,Yuandong Cui,Haoxi Ben,Xiaoli Yang
The sustainable conversion of cellulose to C2 alcohols (ethylene glycol and ethanol) represents a promising sustainable pathway to reduce reliance on fossil resources. However, achieving an effective balance between hydrolysis, C–C bond cleavage, and hydrogenation has remained a challenge. In this study, Pd/WOx catalysts with tunable Pd nanoparticle sizes (1.81–4.46 nm) were developed to investigate the structure–performance relationship. Catalytic evaluations revealed a volcano-type correlation between Pd particle size and C2 alcohol selectivity, with the 3Pd/WOx catalyst, featuring Pd nanoparticles averaging ∼3.0 nm, achieving a maximum selectivity of 78.5% under mild conditions (water solvent, 230 °C, 5 MPa H2, 4 h). Structural and chemical analyses revealed that smaller Pd clusters retained excess oxygen vacancies but lacked hydrogenation capacity, while larger Pd nanoparticles reduced accessible hydrogenation sites and acidity. Mechanistic studies showed that WOx oxygen vacancies promoted cellulose hydrolysis, Pd–O(H)–W sites facilitated glucose adsorption and C–C cleavage to glycolaldehyde, and adjacent Pd0 sites enabled efficient hydrogenation. This work highlights the critical role of Pd particle size in optimizing acid–hydrogenation synergy, providing a green and efficient strategy for biomass valorization without additives or toxic solvents.
研究领域:
催化
·
纳米技术
·
绿色化学
·
生物质转化
·
材料科学
✓ 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）