Molecular Catalysis
·
2023
·
IF 4.6
Xuewu Ji,Guirong Bao,Peng Gao,Jia Luo,Dequan Chen,Zhen Fang
Vanillin hydrodeoxygenation (HDO) was studied in water and methanol using palladium-decorated carbon dots (Pd/CDs). The catalyst was synthesized from photo-reduction of palladium acetate using CDs as the reducing and dispersion agent, while CDs were produced via microwave treatment of glucose and urea. Pd/CDs were characterized with XRD, TEM, FT-IR, XPS, BET and ICP-OES. The selectivity to 2‑methoxy-4-methylphenol (MMP), at vanillin conversion of 100 % after 4.0 h was 98.8 % at 140 °C under 4.0 MPa of H 2 in water with 4.58 wt.% of Pd/CDs. The stability of Pd/CDs was also investigated after four times recycle under the optimal reaction conditions. CDs supported Pd reduced with NaBH 4 and hydrazine hydrate (Pd/CDs-S and Pd/CDs-H) and other carbonaceous materials (active carbon and OH functionalized multi-walled carbon nanotube) supported Pd (Pd/AC and Pd/CNTs) were also investigated for comparison. The highest selectivity to MMP achieved by Pd/CDs produced via photoreduction brings a novel use of this type of catalyst in the conversion of biomass into value-added chemicals and materials.
研究领域:
化学工程
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催化材料
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Changzhou Chen,Wei Chen,Mengqing Zhou,Yongzhi Xiong,Xialin Ji,Minghao Zhou,Liangliang Zhang,Xiaoping Rao,Jianchun Jiang
Large amount of lignin was produced annually as a byproduct in papermaking and pulping processes, the challenges in disposal methods had posed serious obstacles for advanced carbon materials and value-added chemicals. This study involved the preparation of kraft lignin (KL) loaded metal–organic framework (ZIF-67) material derived Co nanoparticles carbon using various methods to produce kraft lignin biochar-based carbon materials (Co@NPC-KLB). The novel and advanced carbon materials was utilized for lignin derived bio-oil hydrodeoxygenation to generate high value fuels and chemicals. It could achieve nearly 100 % vanillin (VAN) conversion and 88.49 % 2-methoxy-4-methylphenol (MMP) without the extra hydrogen at 240 °C in ethanol. The results demonstrated that highly active and stable Co nanoparticles, large specific surface area, smaller nano Co nanoparticles, strong metal-support interaction and rich Lewis acid sites on the surface of biochar support exhibited a positive promoting effect on VAN hydrodeoxygenation to generate MMP. Furthermore, density functional theory (DFT) also confirmed that synergistic effect of Co nanoparticles and kraft lignin biochar promoted a high adsorption energy of VAN on the surface of kraft lignin biochar, enhanced the catalytic ability of the hydrodeoxygenation process. This study provided a novel approach for utilizing kraft lignin in preparation functional catalysts, opening up new opportunities for designing efficient biochar-based materials for advanced carbon materials and high-value chemicals.
研究领域:
材料科学
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催化化学
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生物质转化
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DOI
高影响因子
INORGANIC CHEMISTRY COMMUNICATIONS
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2024
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IF 4.4
Changzhou Chen,Xialin Ji,Jie Jiang,Jianchun Jiang
A range of carbon-encapsulated non-precious metal catalysts (Ni@C, Ce@C, Mo@C, and Zn@C) were prepared using the hydrothermal approach for the catalytic transfer hydrodeoxygenation of vanillin compound derived from lignin. The catalytic efficacy was affected by the level of acid sites, catalyst durability, and the cooperation with H-donor solvents. Analysis indicated that the thin carbon layer enclosing the active sites notably improved catalytic effectiveness and thermodynamic stability compared to alternative catalysts. Notably, Ni@C demonstrated superior catalytic performance, achieving a vanillin conversion rate of 98.72 % and an 87.12 % yield of the major product 2-methoxy-4-methylphenol under specific conditions (240 ℃, 2.0 MPa N 2 , ethanol as a solvent, 4-hour reaction time). These findings underscore the significant potential of carbon-wrapped MOF catalysts in advancing the sustainable utilization of lignin and fostering the growth of a more eco-friendly bioeconomy.
研究领域:
化学工程
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催化科学
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可再生资源利用
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DOI
高影响因子
RSC Advances
·
2021
·Vol. 11
·期 18
·10996-11003
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IF 3.361
Mingxing Duan,Qingyan Cheng,Mingming Wang,Yanji Wang
A new noble metal-free Ni–Co–P/HAP (hydroxyapatite) amorphous alloy catalyst was synthesized by an impregnation-chemical reduction method; the structure and properties of the catalysts were characterized by XRD, SEM, BET, XPS and DSC. Based on the model of the hydrodeoxygenation (HDO) of vanillin to 2-methoxy-4-methylphenol (MMP) with formic acid as a hydrogen source, the catalytic performance of the catalyst was studied. The results found that the Ni–Co–P/HAP catalyst exhibited excellent catalytic activity for the in situ HDO reaction of vanillin compared with Ni–P and Ni–Co–P. The conversion of vanillin could be high to 97.86% with MMP selectivity of 93.97% under optimized reaction conditions. In addition, mechanism studies have shown that the side reaction of carbocation and vanillyl alcohol (HMP) condensation can be effectively reduced with increasing the hydrogenation rate, thereby the selectivity of MMP was effectively increased.
研究领域:
催化化学
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能源化学
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DOI
PubMed
高影响因子
FUEL
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2022
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IF 8.035
Zaiman Zhang,Hao Xu,Hao Li
Hydrodeoxygenation (HDO) in aqueous phase is green and efficient approaches to convert the biomass and its derivative to high value-added chemicals and renewable fuels. However, it remains a great challenge for synthesizing catalysts with the excellent hydrodeoxygenation performance. Three kinds of Ni/Nb 2 O 5 catalyst with different crystal structures (Ni/TT-Nb 2 O 5 , Ni/T-Nb 2 O 5 , Ni/H-Nb 2 O 5 ) were prepared for vanillin hydrodeoxygenation. Compared with the Ni/TT-Nb 2 O 5 and Ni/H-Nb 2 O 5 catalyst, the Ni/T-Nb 2 O 5 catalyst had the most concentration of oxygen vacancies (O v ), which resulted in the excellent hydrodeoxygenation performance. At 180 ℃, 1 MPa H 2 , and the water/ethanol ratio of 8/12, 96.1% conversion of vanillin and 79.2% selectivity of 2-methoxy-4-methylphenol (MMP) were obtained. The abundant O v of Ni/T-Nb 2 O 5 adsorbed and activated the C-OH bonds of vanillyl alcohol (VA), while water formed a stronger transition state with VA to further reduce the disassociation energy of C-OH bonds. The synergistic effect between O v and water promoted the hydrodeoxygenation of vanillin in aqueous phase, achieving the high yield of MMP. This work provides a new idea for the preparation of catalysts with high catalytic performance in aqueous phase.
研究领域:
催化化学
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生物质转化
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绿色化学
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DOI
高影响因子
JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY B-BIOLOGY
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2015
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IF 2.96
Junhui Pan,Langhong Wang,Guowen Zhang,Deming Gong
The characteristics of binding of 2-tert-butyl-4-methylphenol (TBMP), a synthetic phenolic antioxidant with hydroxypropyl-β-cyclodextrin (Hp-βCD) and calf thymus DNA (ctDNA) were investigated by multi-spectroscopic techniques and molecular simulation. The results indicated that TBMP preferred to form a 1:1 inclusion complex with Hp-βCD, with an inclusion constant of determined to be 7.15 × 10 3 L mol −1 . The intercalative mode of TBMP to ctDNA was supported by ctDNA melting temperature and relative viscosity studies, salt quenching effect, competitive binding with methylene blue and molecular modeling. The changes in Fourier transformed infrared (FT-IR) and circular dichroism (CD) spectra suggested that TBMP mainly bound to the G–C rich region with inducing a significant perturbation in B-like DNA structure. It was also found that Hp-βCD decreased the binding ability of TBMP with ctDNA, but did not affect the interactive mode between TBMP and ctDNA, and the formed inclusion complex of TBMP–Hp-βCD decomposed in the presence of ctDNA. This study may provide insights into the mechanism of binding of TBMP with ctDNA and the role of Hp-βCD in the TBMP–ctDNA interaction.
研究领域:
生物化学
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分子生物学
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DOI
PubMed
高影响因子
Catalysts
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2023
·Vol. 13
·期 6
·1002
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IF 3.9
Qi Wu,Dejin Zhang,Shu Sun,Chengcheng Liu,Cong Wang
The synthesis 2-tert-butyl-4-methylphenol is of great significance because of its wide application in industry, and the development of a highly efficient catalyst is necessary for the alkylation of p-cresol and tert-butyl alcohol. Here, an efficient and mild method was established. Caprolactam was chosen as the hydrogen-bonding acceptor; p-toluenesulfonic acid was employed as the hydrogen-bonding donor, and a deep eutectic solvent (DES) was prepared to catalyze the alkylation reaction. The structure of the deep eutectic solvent catalyst was characterized by1H NMR spectra, thermogravimetric analysis, and Fourier transform infrared spectra (FT-IR). In addition, response surface design based on the Box–Behnken method was employed to optimize the alkylation reaction process parameters, and the study of reaction kinetics was also carried out subsequently. The recycle performance of the catalyst was evaluated by recovery experiments, and a good result was obtained. By drawing comparisons with the literature reported, we provide a mild method for the synthesis of 2-tert-butyl-4-methylphenol.
研究领域:
化学工程
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催化化学
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DOI
高影响因子
ChemSusChem
·
2017
·Vol. 11
·期 5
·959-964
·
IF 7.226
Liang Jiang,Peng Zhou,Chanjuan Liao,Zehui Zhang,Shiwei Jin
Graphical Upgrade in progress : Cobalt nanoparticles supported on nitrogen-doped carbon (Co/N-C-600) exhibit high activity for the deoxygenation of vanillin into 2-methoxy-4-methylphenol (MMP) under mild conditions. Nearly quantitative MMP yield is obtained in isopropanol after 8 h at 150 °C and 10 bar H 2 pressure. Moreover, the Co/N-C-600 catalyst also demonstrates high stability. A new method has been developed for the deoxygenation of vanillin to produce 2-methoxy-4-methylphenol (MMP) as a promising liquid fuel over a heterogeneous non-noble metal catalyst. Cobalt nanoparticles supported on nitrogen-doped carbon (Co/N-C-600) exhibit high activity and stability for the deoxygenation of vanillin into MMP under mild conditions (150 °C, 10 bar H 2 ). Nearly quantitative MMP yield is obtained in isopropanol after 8 h at 150 °C and 10 bar H 2 pressure. According to the distribution of products with time, the deoxygenation of vanillin into MMP mainly proceeds through the hydrogenation of vanillin into vanillyl alcohol and the subsequent hydrogenolysis of vanillyl alcohol into MMP, of which the latter is the rate-determining step, owing to a much higher activation energy. Moreover, after being recycled several times, the loss of catalytic activity is negligible, which demonstrates that the Co/N-C-600 catalyst shows good resistance to deactivation.
研究领域:
化学工程
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催化材料
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DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
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IF 3.9
Changyong Li,Mengqing Zhou,Yun Zheng,Shengchun Hu,Liangliang Zhang,Changzhou Chen,Jianchun Jiang
In this study, a series of puffball carbon-supported catalysts were synthesized to facilitate the hydrodeoxygenation (HDO) of the lignin model compound vanillin (VAN) into 2-methoxy-4-methylphenol (MMP). The Co-ZIF/BC catalyst, prepared by loading ZIF-67 onto puffball carbon support, achieved a VAN conversion rate of 96.28% and a selectivity of 86.57% for MMP under reaction conditions of 240 °C and 1.5 MPa of H2 for 4 h. Based on the characterization results, it was found that the Co-ZIF/BC catalyst exhibited high crystal defects, a large specific surface area, and mesopore volume, as well as strong Lewis acid sites. Additionally, the Co–N bonds formed between Co nanoparticles and nitrogen increased the electron density on the catalyst surface. The abundant surface Co0 species enhanced hydrogen adsorption and dissociation, providing more active sites, which facilitated the activation of reactants and improved the efficiency of the catalytic reaction. The use of abundant and low-cost puffball materials in the preparation of the Co-ZIF/BC catalyst not only reduced production costs but also supported the sustainability of the catalytic process, aligning with the principles of green chemistry.
研究领域:
催化化学
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环境科学
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绿色化学
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DOI
高影响因子
ChemCatChem
·
2022
·Vol. 14
·期 14
·e202200397
·
IF 5.497
Jiansu Ran,Lujain Alfilfil,Jingwei Li,Ruixue Yangcheng,Zhaohui Liu,Qin Wang,Yuntong Cui,Tong Cao,Min Qiao,Kexin Yao,Daliang Zhang,Jianjian Wang
Graphical Creation of interfacial microenvironment between Pd nanoparticles and acidic sites greatly enhanced the efficiency in the chemoselective hydrodeoxygenation of vanillin to 2-methoxy-4-methylphenol. Efficient low-temperature hydrodeoxygenation (HDO) of lignin derivatives to produce biofuels and high value-added chemicals is still of challenge. Here, we have constructed a high active and stable 0.2 wt.% Pd/MS-HZSM-5(30) catalyst, and 94.7 % yield of 2-methoxy-4-methylphenol (MMP) can be achieved in HDO of vanillin (VAN, a typical platform molecule of lignin derivatives) under milder reaction conditions (60 °C, 5 h, molar ratio of VAN/Pd=1200, water phase), outperforming the most works reported recently. Detailed experimental and mechanistic studies demonstrated that the superior catalytic performance was due to the rapid hydrogenolysis of generated intermediate (vanillyl alcohol, VAL) to MMP proceeded in an interfacial microenvironmental created by Pd NPs and acidic sites in Pd/MS-HZSM-5(30). These new insights will provide potential guidance for the efficient low-temperature production of biofuels and valuable chemicals from lignin derivatives or raw lignin.
研究领域:
催化化学
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生物质转化
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绿色化学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Jun Wu,Ming Jin,Yong Li,Junfeng Zhao,Tingting Wang,Yuhang Xie,Liqian Liu,Chengbing Wang,Fuwei Li
Catalytic hydrodeoxygenation (HDO) of lignin-derived bio-oils to value-added biofuels is of great importance to efficient utilization of renewable biomass. Precisely tailoring the surface microenvironment of supported metal nanocatalysts plays a significant role in regulating the interaction between reactants and catalytic active sites and facilitates the acquiring of high-performance HDO catalysts for lignin upgrading. Herein, we report a step-economic synthesis of N-doped hollow carbon sphere encapsulated with Co nanoreactors (Co@NHCS-X, X: 700-1000) via the template-directed in-situ crystallization of Co-based ZIF-67 (zeolite imidazolate framework) and pyrolysis process. The optimized Co@NHCS-900 nanocatalyst presented a 100% conversion and 96% selectivity towards valuable 2-methoxy-4-methylphenol (MMP) biofuel through HDO of bio-oils-based vanillin. Such excellent catalytic performance was attributed to the specific structure properties and surface microenvironment of Co@NHCS nanocatalysts. It was demonstrated that the electronic interaction between embedded Co nanoparticles and surface nitrogen species of NHCS nanoreactors constructed desired microenvironment and generated abundant surface Co active species, which could effectively enhance activation capabilities of reactants and intermediate, and achieve highly selective HDO of vanillin to MMP via promoted adsorptions of C O/C O bonds as confirmed by intrinsic kinetic evaluations and density functional theory (DFT) calculations. Moreover, a two-step of hydrogenation/hydrogenolysis tandem reaction pathway of vanillin HDO to MMP and the corresponding catalytic reaction mechanism were proposed. Besides, the hierarchical porous structure of NHCS facilitated the dispersion and stabilization of encapsulated Co nanoparticles and endowed Co@NHCS-900 nanocatalyst with good stability in recycling tests. This work provided new insights into rational design of efficient and stable metal nanocatalysts for biomass conversion.
研究领域:
化学工程
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材料科学
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可再生资源利用
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Changzhou Chen,Xialin Ji,Yongzhi Xiong,Jianchun Jiang
Exploring an advanced catalytic strategy for the high value utilization of lignin derived chemicals into value-added aromatics has attracted tremendous sights for green manufacturing. In this paper, a series of bifunctional 3D rod-shaped mesoporous NiCe metal–organic framework catalysts coupling with hydrogen-donner solvent were reported for the hydrodeoxygenation of vanillin to obtain 2-methoxy-4-methylphenol. Under the optimal conditions, 3Ni-Ce/C catalyst realized the highest conversion of vanillin (>95.0 %) and selectivity of 81.4 % in the absence of additional hydrogen pressure. The characterization results indicated that the interaction of metallic Ni and CeO 2 promoted the generation of Ni-CeO 2-x interface and oxygen vacancies (Ov), which could efficiently adsorb and activate aldehyde group of vanillin to obtain reactive intermediates. And then metallic Ni sites activated the hydrogen-donner solvent to form adsorbed H atoms, which then spilled over to the adjacent Ov to stabilized reactive intermediates. Whereafter, bifunctional 3D rod-shaped mesoporous NiCe metal–organic framework catalysts achieved the hydrodeoxygenation upgrading of vanillin to obtain 2-methoxy-4-methylphenol. Density functional theory (DFT) calculations further revealed that the synergistic effect of Ni-CeO 2 and oxygen vacancies promoted the activation and dissociation of aldehyde group bond in vanillin, enhanced the ability of protonation hydrogenolysis. Additionally, 3Ni-Ce/C catalyst displayed robust activity for no less than four recycles, which provided a feasible method for the build of simultaneous utilization of lignin derivates to value-added fuels and chemicals.
研究领域:
化学工程
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材料科学
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催化反应
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）