ChemSusChem
·
2022
·Vol. 15
·期 13
·e202200092
·
IF 9.14
Xiaohong Hu,Zhijian Li,Haiyong Wang,Haosheng Xin,Song Li,Chenguang Wang,Longlong Ma,Qiying Liu
Graphical Ring-opening : Au/ZrO 2 catalysts with excellent ring-opening hydrogenolysis ability are developed for the selective hydrogenolysis of 5-hydroxymethylfurfural and furfural to produce 2-hexanol and pentanol (1-pentanol and 2-pentanol). The Au-O−Zr interfaces with Lewis acid and metal functionalities play key roles for obtaining the target products with high yield. 2-Hexanol (2-HOL) is a versatile biomass-derived platform molecule for synthesis of liquid transportation fuels, lubricants, or detergents. Herein, a one-step preparation of 2-HOL using 5-hydroxymethylfurfural (HMF) as a substrate was reported for the first time. Several Au-based catalysts supported on different metal oxides were prepared to explore the relationship between carrier and catalytic activity. The results showed that the highest 2-HOL yield of 65.8 % was obtained at complete HMF conversion over the 5 %Au/ZrO 2 catalyst. The 5 %Au/ZrO 2 catalyst exhibited excellent durability after five consecutive recycling runs, while confirming its remarkable ring-opening hydrogenolysis on other biomass-derived furanics, furfural, with a total yield of 1-pentanol and 2-pentanol of 67.4 %. The distinguished ring-opening hydrogenolysis performance of the Au/ZrO 2 catalyst originated from a synergistic effect between the interfacial Au-O-Zr oxygen vacancies-induced Lewis acidic sites (activating C−OH/C=O bonds) and metallic Au (activating H 2 ). This work provides a possibility for producing 2-HOL from HMF with high yield, expanding the sustainable application of lignocellulosic biomass.
研究领域:
催化
·
化学工程
·
可再生能源
·
绿色化学
✓ 已验证
DOI
PubMed
高影响因子
FUEL PROCESSING TECHNOLOGY
·
2016
·
IF 3.847
Hui-Gang Wang,Guo-Liang Shi,Feng Yu,Rui-Feng Li
A solid super acid catalyst, S 2 O 8 2 − /ZrO 2 , was prepared by a new synthesis route of one-pot method with ammonium persulfate via vapor phase hydrolysis to improve biodiesel production using expired soybean oil as reactant. Catalysts were characterized by X-ray diffraction (XRD), transmission electron microscope (TEM), and NH 3 -temperature programmed desorption (NH 3 -TPD) to determine the optimum pretreatment conditions and understand the role of the active sites for transesterification . S 2 O 8 2 − /ZrO 2 calcined at 500 °C, which showed an amorphous phase by XRD characterization, was identified as composed of tetragonal phase ZrO 2 microcrystallites by TEM examination. The microcrystallites which anchored more S 2 O 8 2 − had abundant super acid and displayed high catalytic activity in the transesterification under mild reaction conditions. The reaction parameters over the catalyst were optimized and both the conversion of soybean oil and selectivity of biofuel reached 100% under the conditions of 110 °C of reaction temperature, 4 h of reaction time and 20:1 of methanol to oil molar ratio . Moreover, the catalyst showed high stability in the reactions and no sulfur leaching was found in the biodiesel products in cyclic utilization.
研究领域:
化学工程
·
催化
·
生物燃料
✓ 已验证
产品关联
DOI
高影响因子
CATALYSIS TODAY
·
2024
·
IF 5.2
Yanan Jiang,Huayu Sun,Yuzhen Fang,Cuijuan Zhang,Yuan Liu
The sintering issue of Ni nanoparticles seriously limits the practical application of the Ni-based catalysts for CO 2 methanation. This work demonstrates that the La- and Ce- dual-promoted Ni/ZrO 2 shows better durability at 600 ºC and 60000 mL g cat −1 h −1 over 200 h compared with the La- or Ce- single-promoted. The composition and microstructure characterization indicates that the dispersion and sintering resistance of Ni nanoparticles is enhanced with the dual-promoted catalysts. Both depth profile of X-ray photoelectron spectroscopy and density functional theory calculation show that in the La- and Ce- dual-promoted Ni/ZrO 2 , the reduced dissolution of Ce into ZrO 2 lattice and the spread of La on ZrO 2 surface by forming a La 2 O 3 -CeO 2 solid solution improves the dispersion and stability of Ni nanoparticles. This work provides a facile strategy to mitigate the sintering of Ni nanoparticles and thus improve the stability of Ni-based catalysts for CO 2 methanation.
研究领域:
催化
·
材料科学
·
化学工程
·
表面科学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2024
·
IF 6.7
Wenxia Zhang,Hongtao Zhang,Mohamed Abbas,Juan Zhang,Zhijun Huang,Sibudjing Kawi,Jiangang Chen
The advancement of large-scale and environmentally-friendly solid-state synthesis methods is of paramount importance for the production of precipitated catalysts, notably Fe-based catalysts utilized in Fischer-Tropsch synthesis (FTS). In this study, we present an innovative solvent-independent, wastewater-free solid-state approach for the synthesis of highly efficient Fe/ZrO 2 catalysts, elucidating the mechanisms of promotion within this specific methodology. The prepared catalysts underwent rigorous evaluation under industrially-relevant FTS conditions (230–270 °C, 20 bar, and WHSV = 5400 mL/(g cat ⋅h)). A comprehensive suite of characterization techniques was employed to establish the intricate interplay between catalytic activity and structural attributes. We meticulously examined the impact of Na as an alkali promoter and the role of transition metals (Cu and Mn) in enhancing FTS catalytic performance. The catalytic outcomes obtained clearly demonstrate the pivotal role of the synergistic interaction between Mn and Na within the Na-Mn-Fe/ZrO 2 catalyst system in driving the FTS reaction. This synergism significantly enhances FTS performance, yielding an impressive CO conversion rate (89.91 %) while maintaining low selectivity to CH 4 (7.75 %). The incorporation of Mn and Na into the catalyst matrix enhances the dispersion of Fe 2 O 3 , thereby improving the reducibility of Mn/Fe oxides and elevating the electron density on the catalyst surface. These factors facilitate the formation of active Hägg iron carbide (χ-Fe 5 C 2 ), stimulating chain propagation and ultimately leading to the generation of valuable C 5+ hydrocarbon products, which underscores its potential as an optimal candidate for future industrial applications in Fe-based Fischer-Tropsch synthesis.
研究领域:
催化
·
化学工程
·
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Molecular Catalysis
·
2023
·
IF 4.6
Shuxing Zhang,Jiali Zheng,Zhihui Li,Xiaoshu Ding,Yanji Wang
Herein, we reported a green catalytic reaction system for the synthesis of 5-amino-1-pentanol with furfural and ionic liquid hydroxylamine salt as the initial raw material. In addition, the method can obtain 2-furonitrile and furfurylamine in high yields. The reaction system comprises three new reactions, including the reaction of furfural with ionic liquid hydroxylamine salt to synthesize 2-furonitrile, the hydrogenation of 2-furonitrile to prepare furfurylamine, and the hydrogenolysis of furfurylamine to prepare 5-amino-1-pentanol. For the synthesis of 2-furonitrile, ionic liquid hydroxylamine salt (NH 2 OH) 2 ·[HSO 3 - b - mim ]·HSO 4 was prepared. The ionic liquid as co-solvents, catalysts, and hydroxylamine stabilizer has recovery and reusability. For the hydrogenation of 2-furonitrile to furfurylamine, high-efficiency Ru/g-C 3 N 4 catalyst was prepared. For the hydrogenolysis of furfurylamine to 5-amino-1-pentanol, high-efficiency Pt/ZrO 2 catalyst was prepared. Finally, the yield of 5-amino-1-pentanol based on furfural was 48.7%. A potential pathway for preparing drugs from biomass has been identified in this work.
研究领域:
化学工程
·
催化
·
绿色化学
·
有机合成
·
生物质转化
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2025
·
IF 4.3
Xing Yan,Dongren Cai,Meihong Lin,Zhijie Wu,Yegang Xia,Yanmei Cai,Sajid Ali,Kok Bing Tan,Andriambinintsoa Ranaivoson Tojonirina,Hao Sun,Guowu Zhan
The selective hydrogenation of CO 2 to methanol demands precise control of both catalyst architecture and reaction pathways. Here, we design an atomic layer deposition (ALD)-engineered Pd/ZnO/ZrO 2 ternary catalyst with atomic-scale ZnO interlayers to decouple and reconfigure active sites at dual interfaces (Pd-ZnO and ZnO-ZrO 2 ). This interfacial engineering drives a 7-fold enhancement in methanol space–time yield (0.584 vs. 0.084 g MeOH g cat −1 h −1 ) and switches the dominant reaction pathway from CO-mediated to formate-driven selectivity (methanol selectivity remarkably surges from 6 % to 64 %). Multimodal characterization and theoretical calculations reveal that ZnO interlayers orchestrate bifunctional cooperation: activating CO 2 /CO adsorption while suppressing CO/CH 4 formation through electronic effects. Long-term stability study uncovers a dynamic restructuring mechanism, where Pd-ZnO interfaces gradually evolve into PdZn β alloy phases under the reaction conditions. This work establishes ALD-mediated interface design as a generalizable strategy to manipulate reaction networks and methanol selectivity in catalytic CO 2 hydrogenation systems.
研究领域:
催化化学
·
材料科学
·
化学工程
·
可持续能源
·
表面科学
✓ 已验证
产品关联
DOI
高影响因子
RESEARCH ON CHEMICAL INTERMEDIATES
·
2022
·Vol. 48
·期 6
·2627-2640
·
IF 3.134
Wang Guangying,Liang Yan,Song Jian,Xu Kui,Pan Youchun,Xu Xiaolong,Zhao Yu
Co-doped MnCeO x /ZrO 2 catalysts were synthesized by impregnation method and their low temperature deNOx performance were evaluated. The physicochemical properties of the catalysts were studied. The results showed that the doped Co could promote the deNOx performance of MnCeO x /ZrO 2 significantly, and the doped catalyst with the Co/Mn molar ratio of 1:2 possessed the best catalytic performance. Compared with pure MnCeO x /ZrO 2 catalyst, the deNOx efficiency of the optimal 1Co 2 MnCeO x /ZrO 2 was higher to 93% at 100 °C, improved nearly by 17%. The complete removal of NO was achieved at the temperature range of 120–250 °C. The promoted catalytic performance of Co-doped MnCeO x /ZrO 2 catalyst was mainly attributed to the improvement of the catalyst support structure and surface acidity by Co. The catalytic reaction of NO with NH 3 over 1Co2MnCeO x /ZrO 2 catalyst follows both Eley–Rideal mechanism and Langmiur–Hinshelwood mechanism.
研究领域:
催化
·
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2024
·
IF 6.5
Yiming Chen,Chuan Wang,Yi Liu,Qianwen Zhang,Ling Zhou,Yi Zhang
The selectivity and stability of catalysts for methanol synthesis from CO 2 still remain to be enhanced. In this work, we synthesized a series of Pd/ZrO 2 catalysts inversely loaded with various metal oxide promoters (ZnO, In 2 O 3 , and CeO 2 ), those would partially cover Pd metal surface and form some new metal-promoter interface, to explore the nature in the performance of CO 2 hydrogenation to methanol. The catalyst synthesized by this approach could limit the growth of Pd particles during the reduction and form new metal–metal oxide interfaces with different functions of CO 2 hydrogenation, improving the reaction performance of Pd-ZrO 2 catalysts. As a result, the ZnO-Pd/ZrO 2 catalyst exhibited the highest CO 2 conversion (12.0 %), methanol selectivity (95.6 %), and STY of methanol (472 g MeOH kg cat -1 h −1 ), with excellent stability. The results of HRTEM, H 2 -TPR, XPS, and XAFS showed that the ZnO-Pd/ZrO 2 catalyst had the typical Pd-ZnO interface with Pd 2+ species after the H 2 reduction, which could enhance the adsorption and activation of CO 2 . In addition, the in situ DRIFTS and NAP-XPS results implied that the Pd-ZnO interface significantly improved the formation of formate (HCOO*) and methoxy (H 3 CO*) species, which were considered to be the key intermediates of methanol generation, and thus greatly enhanced the selectivity of methanol.
研究领域:
催化
·
化学工程
·
材料科学
·
环境化学
✓ 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）