RENEWABLE ENERGY
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2020
·
IF 6.274
Han Chen,Qiong Xu,Du Zhang,Wenzhu Liu,Xianxiang Liu,Dulin Yin
A series of mesoporous nickel catalysts with different molar ratios of citric acid and nickel nitrate were synthesized via a simple two-step method by solid-state grinding and in-situ reduction; these catalysts were further employed for the catalytic transfer hydrogenation of levulinate esters to γ-valerolactone (GVL) with 2-propanol as the hydrogen donor. The effects of C 6 H 8 O 7 /Ni molar ratios , catalyst dosage, reaction temperature and time on the catalytic performance were investigated. An excellent GVL selectivity of 99.1% and an ethyl levulinate (EL) conversion of 100% could be achieved at 180 °C in 6 h over Ni-1.0 catalyst with a 1.0:1 M ratio of C 6 H 8 O 7 /Ni. The characterization results showed that the Ni-1.0 catalyst was composed of mesoporous metallic Ni bulk and a surface Ni–NiO composite, and the acid sites of NiO played a synergistic catalytic role in producing GVL from EL. The superior mesoporous structure and large surface area of Ni-1.0 increased the atomic utilization rate of nickel metallic active centers. Moreover, Ni-1.0 catalyst could be easily separated and reused ten times, with an EL conversion above 95% remaining in each recycle. This work provids a highly efficient and environmentally friendly catalytic procedure for the conversion of biomass into GVL, a fuel additive compound.
研究领域:
化学工程
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可再生资源与环境科学
✓ 已验证
产品关联
DOI
高影响因子
DIAMOND AND RELATED MATERIALS
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2021
·
IF 3.315
Zhi-Chao Wang,Xin Cai,Kai Li,Yue-Yuan Ye,Zhao-Xia Zhang,Yun-Quan Liu,Duo Wang,Shui-Rong Li
In this work, a suitable solvent (Lithium Bromide Hydrate) was selected and used for the efficient dissolution and carbonization of biomass for the preparation of carbon spheres directly from wood powders by hydrothermal carbonization (HTC), which was so far the first successful attempt of making carbon spheres directly from woody biomass. The impacts of the preparation conditions on the yield and morphology of carbon spheres were carefully studied, and it was found that the yield and degree of carbonization of carbon spheres were positively correlated with the temperature and reaction time. The optimal operation conditions were determined as 170 °C, reaction time 5 h and LiBr concentration 65 wt%. And the produced carbon spheres have an average particle size of 603 nm with a yield of 22.4%. The characterization of carbon spheres revealed that the prepared nanoparticles had excellent spherical morphology and multifunctional groups, which led to a better surface reactivity than the raw material itself. Moreover, levulinic acid (LA) and 5-hydroxymethylfurfural (5-HMF) were found in the liquid phase of the reaction products, indicating the furan derivatives were formed in the HTC process , which demonstrated a great potential of biomass valorisation with this innovative process.
研究领域:
材料科学
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化学工程
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能源科学
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产品关联
DOI
高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2015
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IF 1.098
Song Zhang,Zhibao Huo,Dezhang Ren,Jiang Luo,Jun Fu,Lu Li,Fangming Jin
An efficient conversion of biomass-derived ethyl lactate to 1,2-propanediol (1,2-PDO) over CuO was investigated. Among the catalysts we tested, CuO, Cu 2 O and Co showed excellent catalytic activity for the conversion of ethyl lactate to 1,2-PDO in water, and CuO was more active and gave the best result. The 1,2-PDO yield of 93.6% was achieved when Zn acted as a reductant. The results indicated that in situ formed hydrogen by the oxidation of Zn in water is more effective than gaseous hydrogen, which failed to produce the 1,2-PDO from ethyl lactate. From a practical point of view, the present method may provide a useful route for the production of 1,2-PDO from ethyl lactate.
研究领域:
化学工程
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催化科学
✓ 已验证
DOI
高影响因子
JOURNAL OF THE AMERICAN OIL CHEMISTS SOCIETY
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2017
·Vol. 94
·期 12
·1481-1489
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IF 1.421
Senan Ahmed M.,Zhang Sicheng,Qin Shuhao,Chen Zhuqi,Yin Guochuan
With the rapid depletion of fossil resources, the exploitation of biomass to partly replace fossil resources as the source of carbon in the chemical industry constitutes a promising alternative for the near future. This work introduces catalytic transformation of vegetable oil, i.e., methyl linoleate, to its conjugated esters by a simple Pd(OAc) 2 /Sc(OTf) 3 catalyst, which has extensive applications in industry. It was found that adding non-redox metal ions like Sc(III) to a simple Pd(OAc) 2 catalyst can effectively improve its isomerization activity in toluene/ t -BuOH solvent, whereas Pd(OAc) 2 alone is inactive. Preliminary mechanistic investigations together with previous studies suggested that the in situ-generated heterobimetallic Pd(II)/Sc(III) dimer serves as the key species for methyl linoleate isomerization, and the reaction proceeds by [1,3]-hydrogen shift mechanism involving a formal Pd(II)/Pd(IV) cycle.
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
✓ 已验证
产品关联
DOI
高影响因子
GREEN CHEMISTRY
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2022
·Vol. 24
·期 4
·1570-1577
·
IF 11.034
Ruixue Yangcheng,Jiansu Ran,Zhaohui Liu,Yuntong Cui,Jianjian Wang
Efficient production of high value-added chemicals and biofuels via low-temperature chemoselective HDO of lignin derivatives in water is still a challenge. Here, we construct a low-cost, active and stable Pd/PCE catalyst using phosphoric acid-modified commercial Celite (PCE) as the support, and this catalyst exhibits excellent activity in low-temperature HDO of vanillin as well as other lignin derivatives in water. The superior catalytic performance is due to the presence of P species on the surface of Pd/PCE, accelerating the selective conversion of the intermediate into the final product. Detailed experimental and mechanistic studies reveal that the rapid conversion of the intermediate to the final product proceeds via a free-radical process in an interfacial microenvironment created by intimate interacting between the P species and Pd NPs. The insights of this work provide a new low-cost catalytic system for efficient production of valuable chemicals and future biofuels from lignin derivatives.
研究领域:
化学工程
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催化科学
✓ 已验证
产品关联
DOI
高影响因子
Molecular Catalysis
·
2023
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IF 4.6
Fukun Li,Ronghe Yang,Ziting Du,Jinhang Dai,Xingmin Wang,Ning Li,Xianming Zhang,Yunqi Liu,Haifeng Gong,Zhenping Cai,Junjun Shi
Biochemicals and biofuel derived from biomass conversion have received much attention over past decades. Alkyl levulinates are considered as promising building block chemicals and green fuel additive. This work presents a facile and efficient catalytic strategy for one pot cascade conversion of furfural to alkyl levulinates over rare earth metal trifluoromethanesulfonates (RE(OTf) 3 ) in alcohol without external H 2 . Experimental results demonstrate that RE(OTf) 3 binds to the alcohol ((OTf) 3 -RE-O(H)R), possessing both Brønsted acid and Lewis acid, plays a key role for this cascade process. Meanwhile, the selectivity of alkyl levulinate is closely related to charge density of selected metal ion and the reduction potential of the selected alcohol. Among various tests, Lu(OTf) 3 , possessing the greatest charge density, exhibits the best catalytic activity in the lowest reduction potential of 2-propanol. 100% furfural conversion and 52.8% ispropanyl levulinate yield can be achieved at 190°C within 45 min. This catalyst can be recycled five times by direct vacuum distillation and regenerated by oxidative elimination of formed humins. Besides, a plausible reaction mechanism is also proposed.
研究领域:
化学工程
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生物化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL RESEARCH IN CHINESE UNIVERSITIES
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2023
·
IF 3.1
Xiang Shuang,Guo Yong,Liu Xiaohui,Wang Yanqin
The interface between Au and support has attracted extensive interest because of its unique catalytic ability for hydrogen activation in catalytic hydrogenation/hydrogenolysis reactions. Herein, we create the Au-CoO-O V interface in the 1.0%Au/Co 3 O 4 -Rod-250 catalyst, which could dissociate H 2 via the heterolytic way to yield rich hydride species and achieve excellent catalytic performance in the hydrogenolysis of biomass-derived 5-hydroxymethylfurfural (HMF) to 2,5-dimethylfuran (DMF). The XRD and HRTEM analyses show that Au nanoparticles are uniformly dispersed on CoO-O V surface and in situ DRIFTS spectra show the enhancement of heterolytic dissociation of hydrogen (signals of Au—D and O—D vibration) compared with bare CoO (Co 3 O 4 -Rod-250). This work provides insights for fabricating highly active Au-support catalysts for catalytic hydrogenation/hydrogenolysis reactions.
研究领域:
化学工程
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催化材料科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
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2022
·
IF 9.224
Yun Wang,Haimei Wu,Jiale Wang,Kaiyue Zhang,Yingxin Liu,Zuojun Wei
A highly effective transformation from renewable biomass and its derivatives into high-value-added chemicals and biofuels is important and challenging. Herein, a N-doped mesoporous carbon (NMC)-supported Ru catalyst developed by an incipient wetness impregnation method was reported for the reductive amination of levulinic acid (LA)/esters with amines to N-substituted 5-methyl-2-pyrrolidinones. A complete conversion of LA with a 99.8% yield of N-hexyl-5-methyl-2-pyrrolidinone (HMP) was achieved over 0.05 mol % Ru/NMC under mild conditions of 120 °C and 1.5 MPa H2 for 4 h, giving a high turnover frequency (3667 h–1). Furthermore, Ru/NMC exhibited superior stability and recyclability (reusable 21 cycles without loss of activity). The excellent performance of the Ru/NMC catalyst was mainly attributed to the introduction of N species to the mesoporous carbon, which not only improved the anchoring and the dispersion of Ru nanoparticles on the catalyst surface but also provided moderate basic sites and transferred electrons from NMC to Ru nanoparticles, as revealed by detailed characterizations. Additionally, the developed Ru/NMC catalytic system was applicable to LA/esters and various amines to afford the corresponding N-substituted 5-methyl-2-pyrrolidinones with excellent yields (80–99%).
研究领域:
催化化学
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可再生化学
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材料科学
✓ 已验证
DOI
高影响因子
RENEWABLE ENERGY
·
2024
·
IF 9
Yanbing Li,Jiayue Ma,Rui Pan,Ting Wang
The efficient use of wood powder has become increasingly important for protecting the environment and addressing energy shortages. In this study, a proton exchange membrane electrolysis system was utilized to convert biomass into valuable industrial chemicals and hydrogen using ferric ions as redox mediators , reduced reaction costs. GC-MC analysis revealed that the degradation products are mainly consisted of aromatic carbonyl compounds , along with some alcohols, phenols , and alkanes. The degradation efficiency was found to be 55.6 %, and the Faraday’s hydrogen production efficiency exceeds 92.6 %. Moreover, Fe 3+ /Fe 2+ redox mediators was recycled in the electrolysis system, maintaining high reactivity. This research introduces a new approach for the degradation of wood powder, offering potential for sustainable industrial production and a reduction in environmental impact.
研究领域:
能源与环境科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Cleaner Production
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2021
·
IF 9.297
Fengjiao Lai,Feng Yan,Pengju Wang,Chunyan Li,Xuehua Shen,Zuotai Zhang
The development of heterogeneously functional catalysts is of great significance in selective catalysis for biomass valorization. Herein, we report for the first time the applicability of chitin/Ag co-modified H 3 PW 12 O 40 composites (Chx-AgPW) as catalysts for producing valuable furans from carbohydrates and biomass. The as-prepared Ch15-AgPW catalyst exhibited the best catalytic performance, due to the dual Brǿnsted-Lewis acidity and appropriate chitin content. When the amount of Ch15-AgPW catalyst was 0.25 mmol, an excellent 5-hydroxymethylfurfural (HMF) yield of 78.3% could be achieved at 150 °C for 3 h with nearly 100% glucose conversion in the H 2 O/MIBK (V H2O:MIBK = 4:6) solvent system. Furthermore, high-yield HMF could also be obtained from other carbohydrates such as fructose (85.3%), sucrose (72.3%), cellobiose (65.6%), starch (52.7%) and inulin (43.5%). Additionally, corn stover , rice straw and sugarcane bagasse under typical reaction conditions simultaneously produced furfural and HMF in yields of 64.6%–72.2% and 18.5%–25.6%, respectively. Combined with the characterization, mechanism study demonstrated that the surface functional groups in chitin were conductive to rapid absorption of the substrates; the Brǿnsted acid sites from heteropoly anion (H 2 [PW 12 O 40 ] - ) promoted the initial depolymerization of biomass and the final dehydration to furans; the introduction of Ag + favored the isomerization of intermediates. After reaction finished, the Ch15-AgPW catalyst could be easily recovered by filtration and effectively reused at least eight cycles without substantial loss in catalytic activity . This work provides a novel strategy to synthesize stable heterogeneous catalysts with tunable acidity for producing bio-based fuels and chemicals from renewable resources .
研究领域:
化学工程
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可再生资源利用
✓ 已验证
产品关联
DOI
高影响因子
ChemCatChem
·
2017
·Vol. 10
·期 6
·1376-1384
·
IF 4.803
Zhaoxia Zheng,Zhicheng Luo,Chen Zhao
Graphical Taking the cross : Morphologically cross-shaped HZSM-5 loaded Ru nanoparticles demonstrate high activity (rate: 7.8 g g −1 h −1 ) in the selective hydrogenolysis of guaiacol to benzene in water with a nearly quantitative yield accompanied with high durability. Hydrogenolysis of C−O bonds is an important tool for synthesis of valuable fuels and chemicals from biomass. In this contribution, we report that morphologically cross-shaped HZSM-5-loaded Ru nanoparticles have demonstrated high activity in the selective hydrogenolysis of guaiacol to benzene in water with 97 % yield and a rate of 7.8 g g −1 h −1 accompanied with high durability. N 2 sorption analysis showed that Ru/HZSM-5 (cross-shaped) had a large mesoporous surface area and pore volume for loading small and uniform Ru nanoparticles, as confirmed by TEM images. The stronger interaction of Ru and cross-shaped HZSM-5 was simultaneously confirmed by a higher hydrogen reduction temperature of RuO 2 on calcined Ru/HZSM-5, a blueshift of Ru δ+ -(CO) n , Ru δ+ -(CO), and Ru 0 -(CO) species in the IR spectra of adsorbed CO, and a higher Ru 3d 5/2 binding energy in X-ray photoelectron spectroscopy measurements. The reaction constant in guaiacol hydrogenolysis to phenol over cross-shaped Ru/HZSM-5 (0.051 min −1 ) was 3–4 times higher than that on spherical and cuboid Ru/HZSM-5 (0.012–0.029 min −1 ) at identical conditions, attributed to the remarkable hydrogenolysis catalytic capability of Ru nanoparticles on cross-shaped HZSM-5. In addition, adsorption of guaiacol and hydrogen was more substantial on cross-shaped Ru/HZSM-5, as evidenced by of IR and mass spectroscopy, respectively. The higher adsorption of guaiacol is attributed to the abundant Lewis acid sites on cross-shaped Ru/HZSM-5, as the Al−OH enriched Lewis acid sites favor the adsorption of oxygen-containing guaiacol. The higher rate constant in the primary step, together with the adsorbed high concentrated reactant and hydrogen (with nearly first-order reaction kinetics) on cross-shaped Ru/HZSM-5, facilitates the overall tandem reaction, leading to an excellent hydrogenolysis catalyst working at hydrothermal conditions for biomass conversion.
研究领域:
催化化学
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能源化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Catalysis
·
2023
·
IF 12.9
Yun Wang,Mengting Chen,Kaiyue Zhang,Haimei Wu,Jiale Wang,Yuran Cheng,Yingxin Liu,Zuojun Wei
Highly efficient transformation of renewable biomass and its derivatives into high-value-added chemicals and biofuels over non-noble-metal catalysts is attractive but challenging. Herein, we developed non-noble CoNi alloy nanoparticles confined in N-doped porous carbon (CoNi@NC) via simple pyrolysis of the metal–organic framework (MOF) precursor at 900 °C under an inert atmosphere. The as-obtained CoNi@NC catalyst exhibited higher performance than monometallic Co@NC and Ni@NC catalysts in the reductive amination of levulinic acid (LA) with benzylamine to N-benzyl-5-methyl-2-pyrrolidinone (BMP) under mild conditions of 130 °C and 3 MPa H2 for 6 h, achieving a full conversion of LA and a ≥ 99% yield of BMP. Detailed characterizations substantiated that multifunctional support and the significant synergistic effect between Co and Ni markedly enhanced the catalytic performance. Furthermore, CoNi@NC manifested outstanding recyclability (reusable 20 cycles without loss of activity), which was attributed to the well-dispersed CoNi alloy nanoparticles confined in the N-doped porous carbon and the anchoring of N species to metal nanoparticles. Additionally, the resultant CoNi@NC catalyst can be successfully applied in the one-pot transformation of LA/esters with amines/nitroarenes/nitriles to the corresponding N-substituted pyrrolidones, as well as the reductive amination of other carbonyl compounds with benzylamine to form N-heterocyclic compounds. Moreover, CoNi@NC enabled us to catalyze the continuous reductive amination of LA with amines in a trickle-bed reactor, which is a more promising, efficient, highly atomically economic, and green synthetic methodology, and exhibited excellent stability during the reaction over 36 h.
研究领域:
化学工程
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材料科学
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催化反应
✓ 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）