RENEWABLE ENERGY
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2024
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IF 9
Xian Shi,Xinyi Xing,Wanni Liu,Mengya Ruan,Ying Guan,Gaojin Lyu,Hui Gao,Siquan Xu
The efficient catalytic conversion of cellulose to 5-hydroxymethylfurfural (HMF) can provide a valuable reference for the high-value utilization of biomass. In this work, a series of simple phosphate-doped hafnium oxide catalysts (x-P-HfO 2 ) were prepared, and their physicochemical properties were analyzed by ICP-OES, XRD, XPS, FTIR, SEM-EDX, N 2 adsorption-desorption isotherms, NH 3 -TPD and Py-FTIR characterizes. Detailed evaluation of the reaction conditions demonstrated the ideal catalytic performance of the x-P-HfO 2 catalysts, and the HMF yield from cellulose reached a satisfactory 61% in the water (NaCl) /tetrahydrofuran biphasic reaction system. Based on the captured intermediates and detected by-products, possible catalytic pathways are summarized. Meanwhile, the hydrothermal stability of the catalyst was also investigated, and the reason for its performance degradation after five cycles was determined to be the loss of useful Brønsted active sites. In addition, the effects of the phosphating and sulfating modification approaches on the catalyst activity were also compared, verifying that the introduction of phosphate is more conducive to the catalyst expressing high activity for the formation of HMF from cellulose.
研究领域:
催化
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生物质转化
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材料科学
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化学工程
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产品关联
DOI
高影响因子
PROCESS BIOCHEMISTRY
·
2024
·
IF 3.7
Cunsheng Zhang,Tianyu Liang,Chengmei Li,Hairui Ji,Hongze Liu,Zhihui Ling,Zhongjian Tian
As a precursor, caproate is widely used in food and medicine for production of various valuable products. From an environmental point of view, caproate production by anaerobic fermentation is a sustainable way. The cost of caproate could be reduced if the wasted biomass is used as substrate. In this study, the caproate production from corn straw and food waste was investigated. Results showed that the sulfuric acid – enzyme method was the optimum approach for hydrolysis of corn straw, and the corresponding glucose concentration was 24.3 g/L. At the optimum condition, the 5-hydroxymethyl furfural (HMF) was found to be the main inhibitor of the hydrolysate, which exhibited inhibitory effect to ethanol and caproate fermentation. Further analysis showed that the inhibition threshold of HMF to Clostridium kluyveri was 1.2 g/L. The formation of biofilm in the fermentation system was found to be an effective way for improving the robustness of cells to inhibitors. The caproate production of 13.5 g/L was obtained when the ethanol and acetate derived from corn straw and food waste was used as substrates. This study cast an insight that it was a promising way for caproate production from the corn straw and food waste.
研究领域:
环境科学
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生物技术
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生物化工
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产品关联
DOI
高影响因子
Frontiers in Chemistry
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2021
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IF 5.221
Jia Hao-Yu,Yang Zi-Yue,Chen Qi,Zong Min-Hua,Li Ning
Catalytic promiscuity is a promising starting point for improving the existing enzymes and even creating novel enzymes. In this work, site-directed mutagenesis was performed to improve promiscuous alcohol dehydrogenase activity of reductive aminase from Aspergillus oryzae (AspRedAm). AspRedAm showed the cofactor preference toward NADPH in reductive aminations, while it favored NADH in the reduction reactions. Some key amino acid residues such as N93, I118, M119, and D169 were identified for mutagenesis by molecular docking. Variant N93A showed the optimal pH and temperature of 8 and 30°C, respectively, in the reduction of 5-hydroxymethylfurfural (HMF). The thermostability was enhanced upon mutation of N93 to alanine. The catalytic efficiency of variant N93A (kcat/Km, 23.6 mM−1 s−1) was approximately 2-fold higher compared to that of the wild-type (WT) enzyme (13.1 mM−1 s−1). The improved catalytic efficiency of this variant may be attributed to the reduced steric hindrance that stems from the smaller side chain of alanine in the substrate-binding pocket. Both the WT enzyme and variant N93A had broad substrate specificity. Escherichia coli (E. coli) cells harboring plain vector enabled selective reduction of biobased furans to target alcohols, with the conversions of 35–95% and the selectivities of >93%. The introduction of variant N93A to E. coli resulted in improved substrate conversions (>98%) and selectivities (>99%).
研究领域:
生物化学
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酶学
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生物催化
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代谢工程
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产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
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2019
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IF 5.155
Cheng Fang,Ping Hu,Shun Dong,Juntao Song,Xinghong Zhang
Smooth, uniform and controllable hydrothermal carbon coatings (HTCCs) had been successfully constructed on the carbon fibers through the efficient hydrothermal transformation approach from renewable carbohydrate. The thickness of HTCC could be effectively tailored from nano-scale to micro-scale by just adjusting the concentration of carbohydrate solution and the oxygen content in the HTCC could be significantly controlled through the high-temperature treatment. As for the growth model of the HTCC, FeCl 3 played a critical role in improving the transformation from glucose to the dehydrated intermediate, mainly composed of 5-hydroxymethylfurfural (HMF), and promoting the conversion from HMF to carbonaceous structure, subsequently. The efficient and scalable preparation route not only offered promising prospects for radically substituting the traditional methods to prepare the carbon coating, but also provided a novel surface modification strategy of carbon fibers in the fields of carbon fiber reinforced composites and flexible textile electronic devices.
研究领域:
材料科学
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化学工程
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纳米技术
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复合材料
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纺织工程
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电子学
✓ 已验证
产品关联
DOI
高影响因子
CATALYSIS TODAY
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2014
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IF 3.309
Songyan Jia,Kairui Liu,Zhanwei Xu,Peifang Yan,Wenjuan Xu,Xiumei Liu,Z. Conrad Zhang
While chromium trichloride hydrate (CrCl 3 ·6H 2 O) effectively catalyzed the isomerization of glucose into fructose in aqueous solution, a general product selectivity behavior was observed independent of reaction variables such as reaction time, temperature, catalyst loading, halide ion, and initial glucose concentration. By studying the mixed solution of dimethylsulfoxide (DMSO) and water at varied DMSO/H 2 O ratios, it was found that deviation from the general water-phase fructose yield curve, with concomitant 5-hydroxymethylfurfral (HMF) formation, occurred when the fructose concentration in available water became sufficiently high in DMSO rich solvent mix. Therefore, tuning the solvent system was the most effective approach to change the product distribution from CrCl 3 ·6H 2 O catalyzed glucose conversion. The apparent activation energy of glucose conversion in the studied system was estimated to be 58.6 kJ mol −1 . Special attention was also given to gain some mechanistic insights by control experiments with simple model compounds and additives, 13 C NMR and UV–vis spectroscopic analyses.
研究领域:
化学工程
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催化
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有机化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of the Taiwan Institute of Chemical Engineers
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2015
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IF 3
Shuguo Wang,Bing Liu,Ziliang Yuan,Zehui Zhang
In this study, magnetic γ-Fe 2 O 3 @ HAP-Mo catalyst was successfully prepared and characterized. The activity of the as prepared γ-Fe 2 O 3 @ HAP-Mo catalyst was evaluated by the oxidation of 5-hydroxymethylfurfural (HMF) with molecular oxygen. Some important reaction parameters were investigated and it was found that both the solvent and the reaction temperature showed great effect on HMF conversion and products selectivity. The highest HMF conversion of 95.8% was obtained in 4-chlorotoluene at the reaction temperature of 120 °C for 12 h, and the corresponding 2,5-diformylfuran, 2,5-furandicarboxylic acid and 5-hydroxymethyl-2-furancarboxylic acid yields were 67.5, 19.6 and 8.7%, respectively. The γ-Fe 2 O 3 @ HAP-Mo catalyst could be easily separated from the reaction mixture and reused several times without the loss of its catalytic activity.
研究领域:
催化
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化学工程
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有机化学
✓ 已验证
DOI
高影响因子
Fundamental Research
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2022
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IF 0
Yingjie Song,Shan Jiang,Yeheng He,Yu Wu,Xin Wan,Wenfu Xie,Jingjing Wang,Zhenhua Li,Haohong Duan,Mingfei Shao
The electrochemical oxidation of biomass molecules coupling with hydrogen production is a promising strategy to obtain both green energy and value-added chemicals; however, this strategy is limited by the competing oxygen evolution reactions and high energy consumption. Herein, we report a hierarchical CoNi layered double hydroxides (LDHs) electrocatalyst with abundant Ni vacancies for the efficient anodic oxidation of 5-hydroxymethylfurfural (HMF) and cathodic hydrogen evolution. The unique hierarchical nanosheet structure and Ni vacancies provide outstanding activity and selectivity toward several biomass molecules because of the finely regulated electronic structure and highly-exposed active sites. In particular, a high faradaic efficiency (FE) at a high current density (99% at 100 mA cm −2 ) is achieved for HMF oxidation, and a two-electrode electrolyzer is assembled based on the Ni vacancies-enriched LDH, which realized a continuous synthesis of highly-pure 2,5-furandicarboxylic acid products with high yields (95%) and FE (90%).
研究领域:
电化学
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催化
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绿色能源
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化工
✓ 已验证
产品关联
DOI
ACS Sustainable Chemistry & Engineering
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2023
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IF 8.4
Guoxing Liu,Huai Liu,Junhua Zhang,Rui Zhang,Heng Zhang,Yong Sun,Lincai Peng
Catalytic conversion of concentrated carbohydrates and raw biomass into 5-hydroxymethylfurfural (HMF), an important and value-added platform chemical, is highly desirable for industrial applications but challenging. In this work, the tin pyrophosphate-oxide (SnP2O7–SnO2) catalyst has been designed to efficiently produce HMF from various concentrated carbohydrates and raw biomass. Especially, a high HMF yield of 67.8% was implemented over the SPC4 catalyst from concentrated glucose (36 wt %) in a biphasic solvent system of water and methyl isobutyl ketone. Moreover, the SPC4 catalyst disclosed a wide range of universality for converting various concentrated carbohydrates and raw biomass to HMF with satisfactory yields (45.9–79.5%). To the best of our knowledge, this is the first example of accomplishing appreciable HMF yields from carbohydrates and raw biomass at such a high substrate concentration. It has been demonstrated that the superior catalytic performance of the catalyst should originate from its balanced Lewis and Brønsted acidity and superhydrophilicity property. This work invents a highly promising heterogeneous catalyst for efficiently valorizing renewable lignocellulose-related compounds into versatile furans.
研究领域:
化学工程
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催化
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可再生能源
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生物质转化
✓ 已验证
产品关联
DOI
高影响因子
Food Chemistry-X
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2024
·
IF 6.5
Ji Wang,Jing Che,Xu-Song Wang,Lei Qin,Xu-Hui Huang
The levels of flavor compounds and hazardous compounds are important indicators for evaluating high-temperature roasted food. In this paper, the effect of tea pre-marination on non-volatile compounds, volatile compounds, and hazardous compounds in roasted chicken. The results showed that the total content of key umami non-volatile compounds in roasted chicken marinated with green tea, white tea, and black tea increased by 17.43 % to 100.11 %. The content of alkenes, alcohols, aldehydes, and ketones in high-temperature roasted chicken marinated with oolong tea and yellow tea was increased. Different teas had varying inhibitory effects on hazardous compounds in high-temperature roasted chicken, while green tea exhibited the highest inhibition efficacy. The inhibition rates of green tea for ACY, 5-HMF, HCAs, and PAHs were 72.12 %, 69.87 %, 92.49 %, and 14.92 %, respectively. Flavonoids in tea may play an important role in the flavor enhancement and hazardous compounds inhibition of high-temperature roasted chicken.
研究领域:
食品科学
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化学
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营养学
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产品关联
DOI
PubMed
高影响因子
INORGANIC CHEMISTRY
·
2024
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IF 4.3
Hongliang Dai,Pengjie Zhou,Shenming Yang,Lili Yang,Hongye Bai,Cui Dai,Guohai Xu,Weiqiang Fan
Electrocatalytic conversion of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) is significant for the sustainable production of value-added chemicals. Active sites of catalysts could enhance the activity and selectivity of the HMF oxidation reaction (HMFOR), but the self-healing ability of active sites has been commonly ignored. In this work, Co(OH)2/Ni-MOF was successfully fabricated for efficient oxidation of HMF to FDCA under mild conditions. Electrochemical and cyclic stability experiments demonstrated the high self-healing properties of the dual active sites (Co3+/Ni3+). So, the retention rate of FDCA yield can still reach 98.5%, even after 90 days. HMFOR was further coupled with 4-nitrophenol hydrogenation, which promotes the yield and Faradaic efficiency of FDCA to about 100%. Therefore, this study explores the self-healing properties of species and provides new insights for designing efficient catalysts.
研究领域:
电化学
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催化
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可持续化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Sustainable Chemistry & Engineering
·
2025
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IF 7.3
Shenghan Gao,Yuting Luo,Bo Li,Wen Cai,Huai Liu,Rui Zhang,Wenlong Jia,Lincai Peng
Modulating the electronic environment of single-atom metal catalysts is a promising yet challenging strategy to optimize their catalytic performance. Herein, electron-rich Ru single atoms were successfully confined within a CoOx matrix (Ru0.6CoOx) through a simple manual grinding-reduction strategy. The resulting Ru0.6CoOx catalyst demonstrated exceptional catalytic activity for the hydrogenolysis of 5-hydroxymethylfurfural (HMF) to 2,5-dimethylfuran (DMF), affording a nearly quantitative DMF yield with an impressive DMF productivity of 210.2 molDMF·mol–1Ru·h–1 at 160 °C. This productivity outperforms most of the noble metal-based catalysts for DMF production. Notably, Ru0.6CoOx also enabled the efficient conversion of HMF to DMF at a low reaction temperature of 120 °C or using a concentrated HMF solution (up to 20 wt %). Experimental studies combined with density functional theory calculations (DFT) revealed that the electronic interaction between the Ru species and CoOx generates electron-rich Ru single atoms, which serve as active sites to boost the H2 activation. Furthermore, the introduction of single Ru atoms was shown to increase the acidity of Ru0.6CoOx, thereby facilitating the cleavage of the C–OH bond during HMF hydrogenolysis. The boosted H2 activation ability and improved acidity of Ru0.6CoOx contribute significantly to its outstanding catalytic performance. This work provides valuable insights into the preparation of electron-rich single-atom metal catalysts for the catalytic hydrodeoxygenation of biomass-derived chemicals.
研究领域:
催化化学
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材料科学
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化学工程
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生物质转化
·
密度泛函理论（DFT）
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Chenhui Xu,Yang Yang,Chengyang Hui,Pengfei Tang,Genlei Zhang,Jialun Liu,Zhenzhen Yang
Highly efficient synthesis of 2,5-diformylfuran (DFF) from 5-hydroxymethylfurfural (HMF) or fructose has attracted much attention in recent years. Herein, one-dimensional MoO2@a-NCx core–shell nanorods that oxygen vacancy-rich molybdenum dioxide (MoO2) coated with porous amorphous nitrogen-doped carbon layer (a-NC) are synthesized via pyrrole polymerization followed by pyrolysis, using orthorhombic molybdenum trioxide (α-MoO3) nanorods as a precursor. Benefiting from the well-engineered architecture and the strong interfacial interaction between MoO2 and surface carbon, the optimized MoO2@a-NC9 with an a-NC layer thickness of ∼9 nm exhibits considerable catalytic activity and stability in oxidation of HMF/fructose to DFF. Under optimal reaction conditions, MoO2@a-NC9 achieves nearly quantitative DFF yield of 99.1% with complete HMF conversion (100%) in the aerobic oxidation of HMF. A possible reaction mechanism involving a Mo4+/Mo3+ redox cycle is proposed for MoO2@a-NC9-catalyzed oxidation of HMF to DFF, based on experimental and characterization results. Furthermore, MoO2@a-NC9 served as a bifunctional catalyst for direct conversion of fructose to DFF via a “one-pot, two-step” approach, achieving a high DFF yield of 82.5%. Notably, this catalyst exhibits excellent recyclability, maintaining its catalytic performance over at least six reaction cycles without significant activity decay.
研究领域:
催化
·
纳米材料
·
绿色化学
·
有机合成
·
能量转换
✓ 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）