Catalysts
·
2020
·Vol. 10
·期 3
·312
·
IF 3.52
Zhiwen Xi,Zhe Hong,Fangtao Huang,Zhirong Zhu,Wenzhi Jia,Junhui Li
A series of Pt/WOx-ZrO2-TiO2catalysts with different Ti/Zr molar ratios was prepared by an evaporation induced self-assembly method, and used to efficient hydrogenolysis of glycerol to 1-PO and 1,3-PDO. BET, XRD, Raman, TEM, XPS and Py-IR were employed to characterize the physicochemical properties of the catalysts. The structural and acidic properties of the catalysts were affected by the Ti/Zr ratio of the support ZrO2-TiO2. Two new crystalline phases of ZrTiO4and Ti2ZrO6and the amount of acid sites were detected in the Pt/WOx-ZrO2-TiO2catalysts. 1-PO is dominant in all products of glycerol hydrogenolysis over the supported Pt-WOx catalysts, which is attributed to more Lewis acid sites on the catalyst surface. The Pt/WOx-ZrO2-TiO2catalyst with a Ti/Zr ratio of 7/3 showed the highest 1,3-PDO yield (25.3%) and 1-PO yield (42.3%), due to its more acid sites including Brønsted and Lewis, and higher concentration of surface Pt0.Keywords:hydrogenolysis of glycerol;1,3-propanediol;1-propanediol;Pt-WOx;ZrO2-TiO2
研究领域:
催化化学
·
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
Frontiers in Chemistry
·
2022
·
IF 5.545
Wang Yaju,Zhou Zhiming,Wang Chao,Zhao Leihong,Xia Qineng
The selective hydrogenolysis of glycerol to 1,3-propanediol (1,3-PDO) with high added value is attraction but challenging. Pt-WOx-based catalysts have been extensively studied in the selective hydrogenolysis of glycerol. The catalyst support and the physicochemical state of WOx play important roles on this reaction. In this paper, Pt-WOx catalysts supported on TiO2 with different crystal forms were prepared and studied for their catalytic performance in hydrogenolysis of glycerol. It was observed that the catalytic performance of anatase-type (A-type) TiO2-supported catalyst (Pt/W/A-Ti) is much better than that of the rutile-type (R-type) TiO2 catalyst (Pt/W/R-Ti) due to its higher stability. Furthermore, the influence of W loading amount and state were thoroughly investigated for the Pt/W/A-Ti catalysts, and Pt/W/A-TiO2 with 5 wt% loading of WOx achieved the best catalytic performance (100% conversion of glycerol and 41% yield of 1,3-PDO under the optimal reaction conditions), owing to the suitable WOx domains and high dispersion of W species, as evidenced by XRD patterns and TEM images. Mechanism study by in-situ DRIFTS experiments indicated that glycerol was first converted to 3-hydroxypropanal and then converted to 1,3-PDO through subsequent reactions.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Xincheng Cao,Shuya Jia,Yao Zhang,Feng Long,Yuwei Chen,Peng Liu,Xiaolei Zhang,Junming Xu,Jianchun Jiang
Fundamental knowledge of the active site requirements for the activation of C−O bonds on heterogeneous catalysts is essential for the design of efficient hydrodeoxygenation catalysts. Pt−WOx (x < 3) catalysts have shown activity and selectivity for the C−O bond breaking of various biomass-derived oxygenates. Yet, the nature of the active sites and the structure−performance relationship have not been well understood because of the intimate coupling of multiple sites. Here, we construct a hybrid catalyst with integrated defective tungsten oxide (e.g., WO2.72) and Pt/C to investigate the role of multiple sites (e.g., metal sites, Bro̷nsted acid, and oxygen vacancy) that are active toward the hydrogenolysis of esters to alkanes in Pt−WOx catalysts. Experimental and theoretical results suggest that oxygen vacancies derived from the defective tungsten oxide (WOx) supply coordinatively unsaturated sites to adsorb and activate the oxygen atom of the carbonyl group of esters, while Pt metal provides an active hydrogen atom for this process. More importantly, it is found that the hydroxyl derived from W−OH in WOx, as a typical Bro̷nsted acid site, can contribute to the adsorption and activation of the C−O bond of esters. The synergistic effect of oxygen vacancies and Bro̷nsted acid sites results in a remarkably efficient acyl C−O bond cleavage of esters, which boosts the hydrodeoxygenation of esters under mild conditions (T ≤ 200 °C). These insights into the structure−performance relationships offer rational methods for designing efficient catalysts for low-temperature hydrodeoxygenation of biomass-derived esters.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Joule
·
2019
·
IF 0
Man Yang,Haifeng Qi,Fei Liu,Yujing Ren,Xiaoli Pan,Leilei Zhang,Xiaoyan Liu,Hua Wang,Jifeng Pang,Mingyuan Zheng,Aiqin Wang,Tao Zhang
Cellulosic ethanol is one of the most important biofuels, yet its commercial production is hindered by the low-efficiency and high-cost bioconversion process. Here, we report a new chemocatalytic approach for the one-pot production of cellulosic ethanol. With a multifunctional Mo/Pt/WO x catalyst, cellulose is directly converted to ethanol in a one-pot reaction with a yield as high as 43.2 C%. Kinetic analysis reveals that such a one-pot process involves tandem catalysis from cellulose to ethylene glycol (rapid) followed by hydrogenolysis of ethylene glycol to ethanol (slow). Characterizations show that isolated and low-coordinated MoO x bonds to metallic Pt particles on the mesoporous WO x support, constituting x OMo–Pt–WO x interfacial sites, which offer high activity for C–O cleavage of ethylene glycol.
研究领域:
化学工程
·
可再生资源与环境科学
✓ 已验证
DOI
危险品化学品经营许可证（带存储）