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
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2018
·
IF 3.525
Man Yang,Xiaochen Zhao,Yujing Ren,Jia Wang,Nian Lei,Aiqin Wang,Tao Zhang
Selective hydrogenolysis of glycerol to 1,3-propanediol (1,3-PD) is an important yet challenging method for the transformation of biomass into value-added chemicals due to steric hindrance and unfavorable thermodynamics. In previous studies, chemoselective performances were found demanding and sensitive to H 2 pressure. In this regard, we manipulate the chemical/physical characteristics of the catalyst supports via doping Nb into WO x and prepared 1D needle-, 2D flake-, and 3D sphere-stack mesoporous structured Nb-WO x with increased surface acid sites. Moreover, Nb doping can successfully inhibit the over-reduction of active W species during glycerol hydrogenolysis and substantially broaden the optimal H 2 pressure from 1 to 5 MPa. When Nb doping is 2%, supported Pt catalysts showed promising performance for the selective hydrogenolysis of glycerol to 1,3-PD over an unprecedentedly wide H 2 pressure range, which will guarantee better catalyst stability in the long run, as well as expand their applications to other hydrogen-related reactions.
研究领域:
催化化学
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生物质转化
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2025
·
IF 4.8
Daguo Wu,Yong Liu,Xinghua Zhang,Jianguo Liu,Qi Zhang,Longlong Ma,Lungang Chen
The effective utilization of biomass is essential for addressing environmental challenges. The direct conversion of cellulose into chemicals and fuels is a key step in fostering a sustainable society. In this study, a mesoporous Pt-WO x /Nb 2 O 5 catalyst is synthesized and characterized using N 2 sorption, XRD, ICP, CO pulse, TEM, SEM, NH 3 -TPD, PY-IR, H 2 -TPR, and XPS. Under optimized catalyst preparation and reaction conditions, the yields of ethanol and propanol reach 50.3 % and 20.2 %, respectively. The mesoporous structure of Nb 2 O 5 , coupled with Pt, provides a rich balance of acidic and hydrogenation-active sites. Additionally, WO x plays a crucial role in the C C bond cleavage of cellulosic glucose and the C O bond cleavage of ethylene glycol, facilitating ethanol formation through Pt and the abundant Lewis acid sites from Nb 2 O 5 .
研究领域:
化学工程
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可再生资源
✓ 已验证
产品关联
DOI
高影响因子
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
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材料科学
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能源化学
✓ 已验证
产品关联
DOI
高影响因子
ENERGY & FUELS
·
2025
·
IF 5.3
Kaixin Jin,Xiao Lu,Zhouwen Li,Guangmai Zhao,Wanpeng Li,Xuewei Zhang,Haiyong Wang,Junzhang Wu,Xiaobin Xie,Li Zhao,Tianhan Zhu,Yuhe Liao,Chenguang Wang,Dalei Zhang
Cellulosic ethanol is a pivotal biofuel, and its chemocatalytic production from lignocellulosic biomass is crucial for addressing global energy challenges. In this study, a series of Pt-loaded catalysts were developed by sequentially loading varying weight percentages (wt %) of Pt and W onto SiO2 carriers using the impregnation method. The catalysts were comprehensively characterized through X-ray diffraction (XRD), high-resolution transmission electron microscopy (HRTEM), X-ray photoelectron spectroscopy (XPS), and Raman spectroscopy to analyze the metal dispersion and active oxidation states on the SiO2 support. Under hydrothermal conditions (240 °C and 4 MPa H2), cellulose was directly converted to ethanol in the aqueous phase, achieving an ethanol yield of 37.5 C%. The catalysts demonstrated excellent stability, maintaining high activity over at least five consecutive reaction cycles. Notably, the WO3 component played a key role in facilitating C–C bond cleavage and hydrolyzing cellulose into glucose and ethanal intermediates. These intermediates were swiftly transferred to the Pt active sites, further promoting the formation of ethylene glycol. Among the catalysts, 3%Pt-15%WO3/SiO2 exhibited optimal performance due to its well-balanced ratios of Pt0 and Pt2+, which enabled selective C–O bond activation and significantly enhanced ethanol production.
研究领域:
生物化学
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催化化学
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可再生能源
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2025
·Vol. 15
·期 18
·14235-14245
·
IF 4.6
Tong Su,Daguo Wu,Xinghua Zhang,Qi Zhang,Lungang Chen,Xiuzheng Zhuang,Longlong Ma
Biomass is an important renewable resource in nature, and cellulose is a crucial component within it. The chemically directed conversion of cellulose into ethylene glycol offers a green alternative to traditional petroleum-based production methods. In this study, a multifunctional Ni–WOx/SAPO-11 catalyst was designed. By optimizing the processing parameters of catalysts and the reaction conditions of them, it was demonstrated that this catalyst could efficiently catalyze cellulose into alcohol products through a series of tandem reactions such as hydrolysis, retro-aldol condensation, and hydrogenation under relatively mild conditions. The yield of ethylene glycol climbed from 4% (at 180 °C) to 66.6% (at 240 °C) with the increase of reaction temperature. Characterization (XPS, TEM, TPD/TPR) revealed that a reduction temperature of 500 °C maximized Brønsted acidity and W5+/W6+ ratios, enhancing C–C cleavage efficiency. Further increases in the reduction temperature would weaken the Brønsted acid on the surface of SAPO-11, but its surface area would also increase (mainly in the form of mesopores). The uniformly dispersed elemental tungsten could form new acidic sites on the catalyst surface; in combination with active Ni0, this high-temperature reduced catalyst could achieve the direct hydrogenolysis of cellulose to produce ethylene glycol, benefiting the efficient utilization of lignocellulosic biomass in the future.
研究领域:
生物质能
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催化化学
·
可再生能源
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Tungsten
·
2024
·
IF 5.6
Weng Yu-Jing,Ding Zhao-Ying,Li Ying-Chao,Wu Yuan-Feng,Xu Yuan-Yang,Chen Rui,Zhao Xiao-Lei,Wang Hai-Yong,Zhang Da-Lei,Zhang Yu-Long
Tungsten and its oxides are highly versatile catalysts with unique properties that hold great promise for a wide array of applications, including biological pathways and chemical processes. The chemo-catalysis of cellulose to ethanol presents a promising avenue for ethanol synthesis with the potential for enhanced efficiency compared to conventional methods, offering a sustainable and carbon–neutral alternative to existing petrochemical and biological processes. Herein, Ir/WO x catalysts enriched with oxygen vacancies were meticulously prepared and demonstrated remarkable catalytic performance in converting cellulose to ethanol directly in the presence of tungstic acid. The catalyst achieved a high ethanol yield of 66.5% under optimal reaction conditions, approaching the theoretical yield limit of traditional ethanol fermentation. Characterization results revealed the presence of oxygen defects, Bronsted/Lewis acidity, and Ir nanoclusters on the catalyst surface, working synergistically to facilitate the cascade catalysis of cellulose hydrolysis, sugar retro-aldol condensation reaction, and C2 intermediate hydrodeoxygenation to ethanol. In situ Fourier transform infrared spectrometer analysis confirmed the catalyst's ability to enhance the adsorption and activation of ethylene glycol for ethanol production. By manipulating subtle structural features, this study offers a fresh perspective on tungsten group catalyst design and underscores the importance of synergistic effects among catalytic sites for the efficient production of ethanol from cellulose.
研究领域:
催化化学
·
可再生能源
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
ChemCatChem
·
2021
·Vol. 13
·期 18
·3953-3959
·
IF 5.686
Zhiming Zhou,Hongyan Jia,Yong Guo,Yangang Wang,Xiaohui Liu,Qineng Xia,Xi Li,Yanqin Wang
Graphical Sulfates : The introduction of sulfates into TiO 2 supported Pt-WO x catalyst greatly improves the dispersion of Pt and WOx species, increases the acid amount and inhibits the leaching of Pt and WO x species, resulting in dramatically promoted catalytic activity and stability for glycerol hydrogenolysis to 1,3-PDO and n-PO with 93 % total yield. Pt-WO x based catalysts were widely investigated and showed high industrial application potential for glycerol hydrogenolysis. Further improving the catalytic activity and stability of the Pt-WO x based catalysts is important. Herein, we modified the TiO 2 supported Pt-WO x catalyst with sulfate doping and employed for the glycerol hydrogenolysis. The introduction of sulfates dramatically promoted the catalytic activity and stability of the Pt/W/Ti catalyst in glycerol hydrogenolysis. Sulfates-doped Pt/W−S/Ti achieved 100 % conversion of glycerol, with 36 % selectivity to 1,3-PDO and 57 % selectivity to n-PO at 120 °C and 4 MPa, while the conversion over Pt/W/Ti only reached 57 %. Moreover, Pt/W−S/Ti offered 22.5 times more glycerol conversion (90 %) than Pt/W/Ti (4 %) for the second run. The much higher activity of the Pt/W−S/Ti was ascribed to the better dispersion of Pt and WO x species and more Brønsted acid amount. The enhanced stability of Pt/W−S/Ti was attributed to its strong anti-leaching ability after sulfate doping.
研究领域:
催化化学
·
工业化学
·
材料科学
✓ 已验证
DOI
高影响因子
ChemCatChem
·
2019
·Vol. 11
·期 16
·3903-3912
·
IF 4.495
Nian Lei,Xiaochen Zhao,Baolin Hou,Man Yang,Maoxiang Zhou,Fei Liu,Aiqin Wang,Tao Zhang
Graphical Pt at it, again ! The highest 1,3-PDO yield was obtained over the Pt/WO x /Al 2 O 3 catalyst with a medium domain size of WO x and a Pt/W atomic ratio of 1/4∼1/2, which favored the dispersion of Pt and maximized the number of Pt−WO x interface sites, and consequently promoted the in-situ production of strong Brønsted acid sites. Selective cleavage of secondary C−O bond is an important yet challenging strategy in glycerol valorization, and the product 1,3-propanediol (1,3-PDO) is of great value in polyester industry. Herein, we report a series of Pt/WO x /Al 2 O 3 catalysts for selective hydrogenolysis of glycerol in a fixed-bed reactor and obtain the highest space-time yield of 1,3-PDO (191.7*10 −3 g 1,3-PDO h −1 g −1 cat. ) to date. Both Pt and W have substantial effects on the 1,3-PDO yield with the optimum Pt/W atomic ratio of 1/2∼1/4. Spectroscopy characterizations as well as chemisorption experiments reveal that at the medium domain size of WO x , hydrogen spillover can take place to the greatest extent due to the improved dispersion of Pt and the suitable reducibility of WO x . Dehydration/dehydrogenation tests of 2-butanol suggest that strong Brønsted acid sites are created via hydrogen dissociation at the Pt−WO x interface and spillover to the neighboring oxygen atom. Such in situ formed protons are critical to the selective cleavage of secondary C−O bonds of polyols.
研究领域:
化学工程
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
Advanced Materials Interfaces
·
2022
·Vol. 9
·期 10
·2102374
·
IF 6.389
Zongtao Liu,Wenjie Lin,Zhiming Chen,Daming Chen,Yifeng Chen,Hui Shen,Zongcun Liang
Nonstoichiometric vanadium oxide V 2 O x has been demonstrated to serve as a hole-selective contact in crystalline silicon solar cells. A reaction between V 2 O x deposited by thermal evaporation and silicon can, however, result in a decreased work function (WF) and reduce hole selectivity. A straightforward and workable solution is presented in this study, which partially restores the WF of V 2 O x as deposited on silicon and improving solar cell efficiency, avoiding the use of amorphous silicon. Incorporating WO x into the Ag/V 2 O x 1 /Si structure, to form Ag/WO x /V 2 O x 2 /Si, x 1 < x 2 , the WF determined by nonstoichiometric ratio, i.e., x , of V 2 O x increases, enhancing the field passivation effect and reducing the rear recombination, which leads to a 11 mV increase in open-circuit voltage and a 0.90 mA cm −2 increase in short-circuit current. Finally, the solar cell gains an absolute improvement of ≈1.0% in power conversion efficiency.
研究领域:
材料科学
·
光伏技术
✓ 已验证
DOI
高影响因子
CATALYSIS LETTERS
·
2022
·Vol. 153
·期 4
·1180-1192
·
IF 2.936
Xing Xiangying,Wang Huixiang,Shi Jing,Li Penghui,Ren Jingzhao,Wang Liancheng,Zhang Jianli,Liu Zhong,Lv Baoliang
WO x has good performance in olefin epoxidation, however, the presence of a large amount of Brönsted acid on WO x affects the selectivity of epoxy products. In this paper, broken carbon spheres ( b-C spheres) treated with nitric acid were used as support to anchor WO x in dynamic solvothermal process. Based on GC–MS and GC-IR detection, the obtained WO x /C greatly increased selectivity of 1,2-epoxyhexane from 16.0% ( pure WO x ) to 92.1% in epoxidation of 1-hexene. The improvement of WO x performance is attributed to the reduction of Brönsted acid sites and electron cloud density after loading, which may all result from interaction between WO x and oxygen-containing functional groups of b-C spheres. Above changes not only effectively inhibit the hydrolysis of 1,2-epoxyhexane, but also are conducive to nucleophilic reaction of H 2 O 2 to WO x, which is beneficial to the activation of H 2 O 2 . Finally, an epoxidation mechanism with oxygen vacancies as the main route under WO x /C catalysis is reasonably proposed. Graphical Abstract
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
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2021
·
IF 3.764
Binbin Zhao,Yu Liang,Wenjun Yan,Lei Liu,Jinxiang Dong
Selective hydrogenolysis of biomass-derived glycerol to 1,3-propanediol (1,3-PDO) is of significant industrial value. The conventional synthetic approach for the supported Pt–WOx catalysts with potential for industrial application generally required a high Pt loading with an aim to create more Pt–O–W interfaces owing to the difficulty in controlling the formation of active WOx species and their high dispersion on supports. In this study, a thin coating of a WOx–Ta2O5 solid solution on a Ta2O5 surface was successfully fabricated by the calcination of W-precursor-containing Ta2O5 at a high temperature (i.e., 900 °C), leading to high dispersion of low-polymeric tungsten oxide with abundant oxygen defects on the support surface. The oxygen defects of the WOx species in the WOx–Ta2O5 solid solution layer played a key role in anchoring and dispersing platinum species to maximize the Pt–O–W interface. WOx(900)/Ta2O5-supported Pt exhibits much higher catalytic efficiency toward the production of 1,3-PDO (TOF1,3-PDO = 23.2 g1,3-PDO·gPt–1·h–1) than that of WOx(500)/Ta2O5-containing Pt derived from routine calcination temperatures. Several characterization techniques were applied to examine the state change of WOx on the support by varying the calcination temperature, as well as the effect of WOx species on the dispersion and chemical states of platinum species.
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
危险品化学品经营许可证（带存储）