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One-pot synthesis of 2,5-bis(hydroxymethyl)furan from biomass derived 5-(chloromethyl)furfural in high yield

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Journal of Energy Chemistry 2023年第1期76卷 421-428,I0011页

作者： Binglin Chen Yunchao Feng Sen Ma Weizhen Xie Guihua Yan Zheng Li Jonathan Sperry Shuliang Yang Xing Tang Yong Sun Lu Lin Xianhai Zeng College of Energy Xiamen UniversityXiamen 361102FujianChina Fujian Engineering and Research Centre of clean and high-valued Technologies for biomass Xiamen Key Laboratory of Clean and High-valued Utilization for BiomassXiamen 361102FujianChina Centre for Green Chemical Science University of AucklandAuckland 1142New Zealand

5-(Chloromethyl)furfural(CMF),as a new platform molecular,has become a hot topic in the field of ***,the one-pot conversion of CMF to 2,5-bis(hydroxymethyl)furan(BHMF)in the water phase was demonstrated for the first time.A 91%BHMF yield was obtained over Ru/Cu Oxcatalyst,and BHMF was mainly produced by the consecutive hydrolysis and hydrogenation of CMF with 5-hydroxymethylfurfural(HMF)as an *** studies revealed that the conversion of HMF to BHMF was the rate-determining ***,the characterizations and density functional theory(DFT)calculations further revealed the lower electron density of Ru NPs in Ru/Cu Oxcatalyst,resulting in a larger adsorption energy and a smaller free energy difference for the formation of *** present findings offered a new pathway for biomass-derived diol production through CMF as a potential source.

关键词： 2 5-Bis(hydroxymethyl)furan Hydrolysis Hydrogenation biomass conversion Heterogeneous catalysis

CAOSA-extracted lignin improves enzymatic hydrolysis of cellulose

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Green Energy & Environment 2024年第7期9卷 1101-1111页

作者： Sen Ma Zheng Li Jonathan Sperry Xing Tang Yong Sun Lu Lin Jian Liu Xianhai Zeng College of Energy State Key Laboratory of Physical Chemistry of Solid SurfacesXiamen UniversityXiamen361102China Fujian Engineering and Research Centre of clean and high-valued Technologies for biomass Xiamen Key Laboratory of Clean and High-valued Utilization of BiomassXiamen361102China Centre for Green Chemical Science University of AucklandAuckland1142New Zealand

The conversion of biomass into sugar platform compounds is very important for the biorefinery *** is essential to the biomass of the sugar platform,however,the lignin obtained by pretreatment,as a key part of lignocellulose,generally has a passive effect on the enzymatic hydrolysis of cellulose into *** this study,p-TsOH(p-toluenesulfonic acid),DES(Deep eutectic solvent)and CAOSA(cooking with active oxygen and solid alkali)pretreatment ways were used to fraction lignin from bamboo *** CAOSA treatment,the hydrolysis efficiency of the pulp was 95.57%.Moreover,the effect of different treatment methods on lignin properties was studied and the promotion effect of lignin was investigated by adding it to the cellulose enzymatic hydrolysis *** this work,the results showed that CAOSA-extracted lignin with lower D(1.31-1.25)had a better adsorption effect on the enzyme protein.p-TsOH-extracted lignin with a larger S/G ratio enhanced the inhibition of enzymatic *** addition,the presence of-COOHs in lignin could reduce its inhibitory effect on cellulose saccharification.

关键词： biomass pretreatment CAOSA Cellulose hydrolysis Lignin Enzyme

Efficient Synthesis of Sugar Alcohols over a Synergistic and Sustainable Catalyst

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Chinese Journal of Chemistry 2021年第9期39卷 2467-2476页

作者： Liangqing Zhang Jiarong Qiu Xing Tang Yong Sun Xianhai Zeng Lu Lin School of Advanced Manufacturing Fuzhou UniversityJinjiangFujian 362251China College of Energy Xiamen UniversityXiamenFujian 361102China Fujian Engineering and Research Center of clean and high-valued Technologies for biomass Xiamen Key Laboratory of High-valued Conversion Technology of Agricultural BiomassXiamen UniversityXiamenFujian 361102China

A series of catalysts were prepared for sugar alcohols production to overcome the deficiencies of the previous reported catalysts,such as low yield of sugar alcohols,single functi on,in stability,and con troversial role of active *** role of each metal and their syn ergistic-cooperati on was discussed in detail with a combi nation of conditional experiments and characterizati *** results indicated that bifunctional *** catalyst has unique structure with superparamagnetism and excellent ***(111)and(200)planes of metallic Ni are the hydrogenation active phases and preferentially exposed on Ni-Al-O_(x) *** desired arabitol or mannitol was obtained by tuning the ratio of Bronsted and Lewis acid *** recycling tests indicated that the unique structure of the prepared Ni-based catalyst can suppress leaching and poisoning,which has high textural stability and activity.

关键词： biomass Heterogeneous catalysis Magnetic properties Br0nsted to Lewis acids Sugar alcohols

Catalyst design strategy toward the efficient heterogeneously-catalyzed selective oxidation of 5-hydroxymethylfurfural

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Green Energy & Environment 2022年第5期7卷 900-932页

作者： Huai Liu Xing Tang Xianhai Zeng Yong Sun Xixian Ke Tianyuan Li Jiaren Zhang Lu Lin biomassChem Group Faculty of Chemical EngineeringKunming University of Science and TechnologyKunming650500China xiamen key laboratory of clean and high-valued utilization for biomass College of EnergyXiamen UniversityXiamen361102China Fujian Engineering and Research Center of clean and high-valued Technologies for biomass Xiamen UniversityXiamen361005China key Lab for Sport Shoes Upper Materials of Fujian Province(Fujian Huafeng New Material Co. Ltd.)Putian351144China PetroChina Petrochemical Research Institute Beijing102206China

The selective oxidation of 5-hydroxymethylfurfural(HMF),a versatile bio-based platform molecule,leads to the formation of several intriguing and useful downstream chemicals,such as 2,5-diformylfuran(DFF),5-hydroxymethyl-2-furancarboxylic acid(HMFCA),formyl 2-furancarboxylic acid(FFCA),2,5-furandicarboxylic acid(FDCA) and furan-2,5-dimethylcarboxylate(FDMC).These products have been extensively employed to fabricate novel polymers,pharmaceuticals,sustainable dyes and many other value-added fine *** heart of the developed HMF oxidation processes is always the *** this regard,this review comprehensively summarized the established heterogeneous catalyst design strategy for the selective oxidation of HMF via *** attention has been focused on the reaction mechanism of HMF oxidation over different catalysts as well as enhancing the catalytic performance of the catalyst through manipulating the properties of the support and fabricating of multi-component metal nano-particles and *** current challenges and possible research directions for the catalytic oxidation of HMF in the future are also discussed.

关键词： hydroxymethyl catalyst catalyzed

Homogenous metallic deposition regulated by abundant lithiophilic sites in nickel/cobalt oxides nanoneedle arrays for lithium metal batteries

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Journal of Energy Chemistry 2023年第2期77卷 11-18,I0001页

作者： Fenqiang Luo Dawei Xu Yongchao Liao Minghao Chen Shuirong Li Dechao Wang Zhifeng Zheng Fujian Provincial Industry Technologies Development Base for New Energy Fujian Provincial Engineering and Research Center of Clean and High-valued Technologies for BiomassXiamen Key Laboratory for High-valued Conversion Technology of Agricultural BiomassCollege of EnergyXiamen UniversityXiamen 361102FujianChina China Fujian Innovation laboratory of Energy Materials Science and Technology(Tan Kah Kee Innovation laboratory) Xiamen 361102FujianChina

Although lithium(Li)metal delivers the highest theoretical capacity as a battery anode,its high reactivity can generate Li dendrites and"dead"Li during cycling,resulting in poor reversibility and low Li *** uniform Li plating/stripping is the core of solving these ***,we design a highly lithiophilic carbon film with an outer sheath of the nanoneedle arrays to induce homogeneous Li plating/*** excellent conductivity and 3D framework of the carbon film not only offer fast charge transport across the entire electrode but also mitigate the volume change of Li metal during *** abundant lithiophilic sites ensure stable Li plating/stripping,thereby inhibiting the Li dendritic growth and"dead"Li *** resulting composite anode allows for stable Li stripping/plating under 0.5 mA cm^(-2) with a capacity of 0.5 mA h cm^(-2) for 4000 h and 3 mA cm^(-2) with a capacity of3 mA h cm^(-2) for 1000 *** Ex-SEM analysis reveals that lithiophilic property is different at the bottom,top,or channel in the structu re,which can regulate a bottom-up uniform Li deposition *** cells paired with LFP show a stable capacity of 155 mA h g^(-1) under a current density of *** pouch cell can keep powering light-emitting diode even under 180°bending,suggesting its good flexibility and great practical applications.

关键词： Nickel/cobalt oxides Nanoneedle arrays Lithiophilic sites Lithium metal batteries

Formation mechanism of solid product produced from co-pyrolysis of Pingdingshan lean coal with organic matter in Huadian oil shale

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Frontiers of Chemical Science and Engineering 2021年第2期15卷 363-372页

作者： Xiangchun Liu Jun Hu Ruilun Xie Bin Fang Ping Cui Anhui key laboratory of Coal clean Conversion&utilization Anhui Province Key Laboratory of Coal Clean Conversion and High Valued UtilizationSchool of Chemistry and Chemical EngineeringAnhui University of TechnologyMa’anshan 243032China

A mixture of Pingdingshan lean coal and acid-treated Huadian oil shale was co-pyrolyzed in a drop-tube fixed-bed reactor in the temperature range of 300℃–450℃.To reveal the formation mechanism of the solid co-pyrolysis product,changes in some physicochemical properties were investigated,using analysis by X-ray diffraction,X-ray photoelectron spectroscopy,scanning electron microscopy,pore analysis,thermogravimetry,and electron spin resonance.X-ray diffraction showed that the lattice plane spacing for the co-pyrolyzed mixture decreased from 0.357 nm to 0.346 nm and the average stacking height increased from 1.509 nm to 1.980 nm in the temperature range of 300°C–450°C,suggesting that pyrolysis treatment increased its degree of *** amount of oxygen-containing functional groups and pore volume decreased with increasing *** and electron spin resonance results showed that synergistic effects occurred during the co-pyrolysis process.A formation mechanism for the solid product was ***-rich radicals generated from the pyrolysis of the oil shale were trapped by hydrogen-poor macromolecular radicals of the intermediate metaplast produced from coal pyrolysis,thereby increasing the yield of solid product.

关键词： co-pyrolysis coal oil shale electron spin resonance mechanism

Heterogeneously-catalyzed aerobic oxidation of furfural to furancarboxylic acid with CuO-Promoted MnO_(2)

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Green Energy & Environment 2023年第6期8卷 1683-1692页

作者： Xin Yu Tingke Jin Huiqiang Wang Guoqing Zhang Wenlong Jia Lincai Peng Yong Sun Xing Tang Xianhai Zeng Shuliang Yang Zheng Li Feng Xu Lu Lin College of Energy Xiamen UniversityXiamen361102China Institute of Geology Xibu Drilling Engineering Company LimitedChina National Petroleum CorporationXinjiang834000China biomassChem Group Faculty of Chemical EngineeringKunming University of Science and TechnologyKunmingYunnan650500China Fujian Engineering and Research Center of clean and high-valued Technologies for biomass China xiamen key laboratory of high-valued utilization of biomass Xiamen UniversityXiamen361102China Beijing Forestry Univ Inst Biomass Chem&TechnolBeijing100083China

A cost-effective and sustainable noble-metal free catalyst system based on ubiquitously available Mn-Cu bimetallic oxides was served as efficient catalysts for furfural selective oxidation to furancarboxylic acid(FA). Interestingly, Mn_(2)Cu_(1)O_(x)exhibited an excellent furfural conversion of 99% with quantitative selectivity toward FA. Especially, we demonstrate the significant weakening of the Mn-O bonds with the incorporation of CuO into the Mn-Cu oxides, resulting in an improved OLreactivity of Mn_(2)Cu_(1)O_(x), which brings about a higher catalytic activity for furfural oxidation. More importantly, Mn_(2)Cu_(1)O_(x)could exhibit YFA>90% over 5 cycles of reusability test. Through this study, the relationship between the morphology, surface chemistry, and catalytic activity of Mn-Cu bimetallic oxides are elucidated, providing a simple and environmentally friendly catalytic strategy and scientific basis for the development of Mn-Cu bimetallic oxides bioderived molecular aerobic oxidation materials.

关键词： Furfural Mn–Cu bimetallic oxides Oxidation Lattice oxygen Furancarboxylic acid

Oxygen-vacancy-rich MnO_(x)supported RuO_(x)for efficient base-free oxidation of 5-hydroxymethylfurfural and 5-methoxymethylfurfural to 2,5-furandicarboxylic acid

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Journal of Energy Chemistry 2024年第8期95卷 670-683,I0015页

作者： Jiali Wu Weizhen Xie Yining Zhang Xixian Ke Tianyuan Li Huayu Fang Yong Sun Xianhai Zeng Lu Lin Xing Tang xiamen key laboratory of clean and high-valued Applications for biomass Fujian Engineering and Research Center of Clean and High-valued Technologies for BiomassCollege of EnergyXiamen UniversityXiamen 361102FujianChina key Lab for Sport Shoes Upper Materials of Fujian Province Fujian Engineering and Research Center for New Functional Fiber Materials(Fujian Huafeng New Material Co.Ltd.Putian Dakai New Material Co.Ltd.)Putian 351144FujianChina

2,5-Furandicarboxylic acid(FDCA)is a promising biomass-derived polymeric monomer that serves as an attractive alternative to terephthalic acid derived from fossil ***,the green and efficient production of FDCA through the oxidation of 5-hydroxymethylfurfural(HMF)and its derivatives is still rudimentary under base-free *** this work,oxygen-vacancy-rich Mn Oxwas prepared and displayed a strong adsorption and anchoring ability to Ru species that mainly exposed the(210)plane of RuO_(2),bringing about highly dispersed and active interfacial Ru-O-Mn *** results and density functional theory calculations confirm that these above features greatly facilitate the adsorption/activation of oxygen and the dehydrogenation-oxidation of HMF/5-methoxymethylfurfural(MMF),which enables an efficient FDCA production under base-free and mild ***,a desirable FDCA yield of 86.56%was still obtained from concentrated HMF(10 wt%)under base-free conditions over oxygen-vacancy-rich Mn Oxsupported Ru Ox(1.0 MPaO_(2),120℃,6 h).This work delineates a facile catalyst preparation strategy for HMF/MMF oxidation,and might open a new avenue for the green synthesis of FDCA under base-free conditions.

关键词： Base-free oxidation Oxygen-vacancy-rich 5-Hydroxymethylfurfural 5-Methoxymethylfurfural 2 5-Furandicarboxylic acid

Effective production of γ-valerolactone from biomass-derived methyl levulinate over CuO_x-CaCO_3 catalyst

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Chinese Journal of Catalysis 2019年第2期40卷 192-203页

作者： Xuejuan Cao Huai Liu Junnan Wei Xing Tang Xianhai Zeng Yong Sun Tingzhou Lei Geng Zhao Lu Lin xiamen key laboratory of clean and high-valued utilization for biomass College of EnergyXiamen UniversityXiamen 361102FujianChina Fujian Engineering and Research Center of clean and high-valued Technologies for biomass Xiamen 361005FujianChina Henan key Lab of biomass Energy Zhengzhou 450008HenanChina College of Chemistry and Chemical Engineering Xinyang Normal UniversityXinyang 464000HenanChina

The production of?-valerolactone(GVL)from lignocellulosic biomass has become a focus of research owing to its potential applications in fuels and *** this study,(n)CuOx-CaCO3(where n is the molar ratio of Cu to Ca)compounds were prepared for the first time and shown to function as efficient bifunctional catalysts for the conversion of biomass-derived methyl levulinate(ML)into GVL,using methanol as the in-situ hydrogen *** the catalysts with varied Cu/Ca molar ratios,(3/2)CuOx-CaCO3 provided the highest GVL yield of 95.6% from *** incorporation of CaCO3 with CuO resulted in the formation of Cu+species in a CuOx-CaCO3 catalyst,which greatly facilitated the hydrogenation of ***,CuOx-CaCO3 also displayed excellent catalytic performance in the methanolysis products of cellulose,even in the presence of ***,a facile two-step strategy for the production of GVL from cellulose could be developed over this robust and inexpensive catalyst,through the integration of cellulose methanolysis catalyzed by sulfuric acid,methanol reforming,and ML hydrogenation in methanol medium.

关键词： γ-Valerolactone Methyl levulinate Hydrocyclization Methanol reforming Cellulose methanolysis