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Plasmonic quantum dots modulated nano-mineral toward photothermal reduction of CO_(2)coupled with biomass conversion

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Nano Research 2024年第6期17卷 5061-5072页

作者： Guangbiao Cao Haoran Xing Haoguan Gui Chao Yao Yinjuan Chen Yongsheng Chen Xiazhang Li National-local Joint Engineering Research Center of biomass Refining and High-quality Utilization Changzhou UniversityChangzhou 213164China School of Civil and Environmental Engineering Georgia Institute of TechnologyAtlantaGA 30332-0373USA

Simultaneous conversion of CO_(2)and biomass into value-added chemicals through solar-driven catalysis holds tremendous importance for fostering a sustainable circular ***,plasmonic Bi quantum dots were immobilized on phosphoric acid modified attapulgite(P-ATP)nanorod using an in-situ reduction-deposition method,and were employed for photocatalytic reduction of CO_(2)coupled with oxidation of biomass-derived benzyl *** revealed that Bi atoms successfully integrated into the basal structure of P-ATP,forming chemically coordinated Bi-O-Si bonds that served as efficient transportation channels for *** incorporation of high-density monodispersed Bi quantum dots induced a surface plasmon resonance(SPR)effect,expanding the light absorption range into the near-infrared *** a consequence,the photo-thermal transformation was significantly accelerated,leading to enhanced reaction ***,50%Bi/P-ATP nanocomposite exhibited the highest plasmon-mediated photocatalytic CH4 generation(115.7μmol·g^(−1)·h^(−1))and CO generation(44.9μmol·g^(−1)·h^(−1)),along with remarkable benzaldehyde generation rate of 79.5μmol·g^(−1)·h^(−1)in the photo-redox coupling system under solar light *** hydrogen protons released from the oxidation of benzyl alcohol facilitated the incorporation of more hydrogen protons into CO_(2)to form key CH_(3)O−*** work demonstrates the synergistic solar-driven valorization of CO_(2)and biomass using natural mineral based catalyst.

关键词： photothermal catalysis clay mineral plasmon CO_(2)reduction biomass conversion

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Torrefied Pellets as Fuel for Two-Stage Technology of biomass conversion into Synthesis Gas

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Journal of Energy and Power Engineering 2014年第1期8卷 79-84页

作者： Victor Zaichenko Valentin Kosov Julia Kuzmina Vladimir Lavrenov JIHT RAS (Joint Institute for High Temperatures of the Russian Academy of Sciences) Moscow 125412 Russia

One of the most important properties of the torrefied pellets, along with high calorific value, is their hydrophobicity. Inability to absorb moisture and self-destruct under its influence determine possibility of using of pellets in the pyrolysis reactor. For the technology of two-stage thermal processing of biomass, developed at the Joint Institute for High Temperatures, the amount of synthesis gas which can be obtained from one kilogram of torrefied pellets is also important. A construction of the pilot torrefaction reactor powered by flue gas is shown. The results of experimental investigations of hydrophobicity of torrefied pellets produced by the reactor and quantity of synthesis gas which can be obtained by two-stage thermal processing of the pellets are presented. It is shown that torrefaction allows simplifying the process of conversion of pellets into synthesis gas without significant reduction in the volume of the gas.

关键词： biomass conversion torrefaction pyrolysis syngas.

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Synthesis and Catalytic Application of Zeolite Supported Metal Nanocatalysts in the conversion of biomass

Synthesis and Catalytic Application of Zeolite Supported Met...

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第18届全国分子筛学术大会

作者：王亮孟祥举肖丰收浙江大学催化研究所

biomass,which is regarded as a renewable feedstock,has attracted much attention for the production of fine chemicals and *** economically viable proc-esses have been developed for the conversion of *** example,it is noted that direct use of the phenolic bio-oils is im-possible,because their high oxygen content lead to low energy density,high viscosity,and low ***,upgrading bio-oils by hydrodeoxygenation is strongly desirable in order to produce high-quality alkane ***,we show that the mesoporous ZSM-5 zeolites（ZSM-5-M）supported Ru nanoparticles are efficient catalysts for the hydrodeoxygenation of phenolic compounds in bio-oil to ***,b-axis-aligned mesoporous ZSM-5（ZSM-5-OM）,a new type of mesoporous zeolite with b-axis-aligned mesopores,supported Ru nanoparticles are very active for the production of alkane bio-oils,because of the open mesopores on ZSM-5-OM with rich exposed acid sites for catalyzing the cleavage of C-O bonds,a key step in the hydrodeoxygenation of phenolic molecules to alkanes.

关键词： zeolite biomass conversion oxidation hydrogenation

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Surface functionalized Pt/SnNb_(2)O_(6)nanosheets for visible-light-driven the precise hydrogenation of furfural to furfuryl alcohol

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Journal of Energy Chemistry 2022年第3期31卷 566-575,I0015页

作者： Yingzhang Shi Huan Wang Zhiwen Wang Cheng Liu Mingchuang Shen Taikang Wu Ling Wu State Key Laboratory of Photocatalysis on Energy and Environment Fuzhou UniversityFuzhou 350116FujianChina State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of ScienceFuzhou 350002FujianChina

Photocatalytic upgrading of renewable biomass is a promising way to relieve energy crisis and environmental ***,low photocatalytic efficiency and uncontrollable selectivity still limit its ***,ultrathin SnNb_(2)O_(6)nanosheets with high dispersed Pt nanoparticles(Pt/SN)were successfully developed as an efficient photocatalyst for the precise hydrogenation of furfural(FUR)to furfuryl alcohol(FOL)under visible light irradiation and exhibited the high conversion of FUR(99.9%)with the high selectivity for FOL(99.9%).It was revealed that SN with only 4.1 nm thickness possess good separation ability of photo-generated carriers and abundant surface Lewis acid sites(Nb^(5+))which would selectively chemisorb and activate FUR molecules via the Nb···O=C ***,Pt nanoparticles would gather photo-generated electrons for greatly promoting the generation of active H species to support the hydrogenation of FUR to *** synergistic effects between SnNb_(2)O_(6)nanosheets and Pt nanoparticles remarkably facilitate the photocatalytic performance for *** work not only confirms the great potential of ultrathin nanosheet photocatalyst with functional metal sites for precise upgrading of biomass but also provides an in-depth view to understand the surface/interface interaction between reactant molecules and surface sites of a photocatalyst.

关键词： biomass conversion Hydrogenation of furfural Two-dimensional materials Sn2NbO6 nanosheet Pt nanoparticle Photocatalysis

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Sustainable Furfural biomass Feedstocks Electrooxidation toward Value-Added Furoic Acid with Energy-Saving H_(2) Fuel Production Using Pt-Decorated Co_(3)O_(4) Nanospheres

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Energy & Environmental Materials 2024年第2期7卷 350-358页

作者： Talshyn Begildayeνa Jayaraman Theerthagiri Seung Jun Lee Ahreum Min Gyeong-Ah Kim Siνakumar Manickam Myong Yong Choi Department of Chemistry(BK21 FOUR) Core-Facility Center for Photochemistry&NanomaterialsResearch Institute of Natural SciencesGyeongsang National UniversityJinju 52828South Korea Petroleum and Chemical Engineering Faculty of EngineeringUniversiti Teknologi BruneiJalan Tungku Link GadongBandar Seri Begawan BE1410Brunei Darussalam

Here,furfural oxidation was performed to replace the kinetically sluggish O_(2)evolution reaction(OER).Pt-Co_(3)O_(4)nanospheres were developed via pulsed laser ablation in liquid(PLAL)in a single step for the paired electrocatalysis of an H_(2)evolution reaction(HER)and furfural oxidation reaction(FOR).The FOR afforded a high furfural conversion(44.2%)with a major product of 2-furoic acid after a 2-h electrolysis at 1.55 V versus reversible hydrogen electrode in a 1.0-M KOH/50-mM furfural *** Pt-Co_(3)O_(4)electrode exhibited a small overpotential of 290 mV at 10 mA cm^(-2).As an anode and cathode in an electrolyzer system,the Pt-Co_(3)O_(4)electrocatalyst required only a small applied cell voltage of~1.83 V to deliver 10 mA cm^(-2),compared with that of the pure water electrolyzer(OER||HER,~1.99 V).This study simultaneously realized the integrated production of energy-saving H_(2)fuel at the cathode and 2-furoic acid at the anode.

关键词： biomass conversion electrochemical furfural oxidation overall water splitting Pt-Co_(3)O_(4)electrocatalyst pulsed laser ablation in liquid

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Cooperative catalysis of Co single atoms and nanoparticles enables selective CAr-OCH_(3) cleavage for sustainable production of lignin-based cyclohexanols

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Journal of Energy Chemistry 2023年第4期79卷 535-549页

作者： Baoyu Wang Peng Zhou Ximing Yan Hu Li Hongguo Wu Zehui Zhang National Key Laboratory of Green Pesticide Key Laboratory of Green Pesticide&Agricultural BioengineeringMinistry of EducationState-Local Joint Laboratory for Comprehensive Utilization of BiomassCenter for R&D of Fine ChemicalsGuizhou UniversityGuiyang 550025GuizhouChina Key Laboratory of Catalysis and Material Sciences of the State Ethnic Affairs Commission&Ministry of Education College of Chemistry and Material SciencesSouth-Central University for NationalitiesWuhan 430074HubeiChina Guangxi Key Laboratory of Green Chemical Materials and Safety Technology Beibu Gulf UniversityQinzhou 535011GuangxiChina College of Pharmacy Guizhou UniversityGuiyang 550025GuizhouChina

In this work,a dual-size MOF-derived Co catalyst(0.2Co_(1-NPs)@NC)composed of single atoms(Co_(1))and highly dispersed nanoparticles(Co NPs)was prepared by in-situ Zn evaporation for the highperformance conversion of lignin-derived o-methoxyphenols(lignin oil)to cyclohexanols(up to 97%yield)via cascade demethoxylation and *** calculations elaborated that the dual-size Co catalyst exhibited a cooperative effect in the selective demethoxylation process,in which the Co NPs could initially dissociate hydrogen at lower energies while Co1remarkably facilitated the cleavage of the C_(Ar)-OCH_(3)***,the intramolecular hydrogen bonds formed in the omethoxy-containing phenols were found to result in a decrease in the bond energy of the C_(Ar)-OCH_(3)bond,which was more prone to be activated by the dual-size Co ***,the pre-hydrogenated intermediate(e.g.,2-methoxycyclohexanol from guaiacol)is difficult to undergo demethoxylation,indicating that the selective C_(Ar)-OCH_(3)bond cleavage is a prerequisite for the synthesis of *** 0.2Co_(1-NPs)@NC catalyst was highly recyclable with a neglect decline in activity during five consecutive *** cooperative catalytic strategy based on the metal size effect opens new avenues for biomass upgrading via enhanced C-O bond cleavage of high selectivity.

关键词： biomass conversion Heterogeneous catalysis C-O bond cleavage Lignin valorization Cyclohexanols

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Identification of the hydrogen utilization pathway for the electrocatalytic hydrogenation of phenol

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Science China Chemistry 2021年第9期64卷 1586-1595页

作者： Ling Zhou Xiaorong Zhu Hui Su Hongzhen Lin Yanhong Lyu Xu Zhao Chen Chen Nana Zhang Chao Xie Yingying Li Yuxuan Lu Jianyun Zheng Benrt Johannessen San Ping Jiang Qinghua Liu Yafei Li Yuqin Zou Shuangyin Wang State Key Laboratory of Chem/Bio-Sensing and Chemometrics Provincial Hunan Key Laboratory for Graphene Materials and DevicesCollege of Chemistry and Chemical Engineeringthe National Supercomputer Centers in ChangshaHunan UniversityChangsha410082China College of Chemistry and Materials Science Nanjing Normal UniversityNanjing210023China National Synchrotron Radiation Laboratory University of Science and Technology of ChinaHefei230026China i-LAB Suzhou Institute of Nano-Tech and Nano-Bionics(SINANO)Chinese Academy of SciencesSuzhou215123China Department of Educational Science Hunan First Normal UniversityChangsha410205China Australian Synchrotron ClaytonVictoria3168Australia Western Australian School of Mines:Minerals Energy and Chemical Engineering and Fuels and Energy Technology InstituteCurtin UniversityPerthWA6102Australia

Electrochemical hydrogenation(ECH)of biomass-derived platform molecules is a burgeoning route for the sustainable utilization of ***,the noble-metal-catalyzed ECH of phenolic compounds suffers from intense competition with hydrogen evolution *** prepared Pt Rh bimetallic nanoparticles dispersed on highly ordered mesoporous carbon nanospheres,which improves the utilization efficiency of adsorbed hydrogen(H_(ad))to ECH in H-UPD region(>0 V ***).Further analysis reveals(i)the strong overlapping between the d-orbitals of Pt and Rh enhances specific adsorption of phenol;(ii)incorporation of Rh devotes an electronic effect on weakening the alloy-H_(ad)interaction to increase the FE of *** calculations confirm the selectivity difference and the ECH parallel pathways:cyclohexanol and cyclohexanone are formed via hydrogenation/dehydrogenation of the intermediate ^(*)C_(6)H_(10) *** findings deepen our fundamental understanding of the ECH process,and cast new light on exploration of highly efficient electrocatalysts for biomass upgrading.

关键词： electrohydrogenation aromatic hydrogenation biomass conversion Pt Rh alloy

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Mesoporous zeolites for biofuel upgrading and glycerol conversion

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Frontiers of Chemical Science and Engineering 2018年第1期12卷 132-144页

作者： Jian Zhang Liang Wang Yanyan Ji Fang Chen Feng-Shou Xiao Key Laboratory of Applied Chemistry of Zhejiang Province and Department of Chemistry Zhejiang University Hangzhou 310028 China Key Laboratory of biomass Chemical Engineering of Ministry of Education Zhejiang University Hangzhou 310027 China

With the recent emphasis and development of sustainable chemistry, the conversion of biomass feed- stocks into alternative fuels and fine chemicals over various heterogeneous catalysts has received much attention. In particular, owing to their uniform micropores, strong acidity, and stable and rigid frameworks, zeolites as catalysts or co-catalysts have exhibited excellent catalytic performances in many reactions, including hydrodesulfurization, Fischer-Tropsch synthesis, and hydrodeoxygenation. However, the relatively small sizes of the zeolite micropores strongly limit the conversion of bulky biomolecules. To overcome this issue, mesoporous zeolites with pores larger than those of biomolecules have been synthesized. As expected, these mesoporous zeolites have outperformed conventional zeolites with improved activ- ities, better selectivities, and longer catalyst lives for the upgrading of pyrolysis oils, the transformation of lipids into biofuels, and the conversion of glycerol into acrolein and aromatic compounds. This review briefly summarizes recent works on the rational synthesis of mesoporous zeolites and their superior catalytic properties in biomass conversion.

关键词： biomass conversion mesoporous zeolite sustainable chemistry

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Engineering active Ni-doped Co_(2)P catalyst for efficient electrooxidation coupled with hydrogen evolution

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Nano Research 2023年第5期16卷 6728-6735页

作者： Jiayi Li Xin Mao Wanbing Gong Xinyu Wang Yawen Jiang Ran Long Aijun Du Yujie Xiong National Synchrotron Radiation Laboratory Hefei National Research Center for Physical Sciences at the MicroscaleSchool of Chemistry and Materials ScienceUniversity of Science and Technology of ChinaHefei 230026China Institute of Energy Hefei Comprehensive National Science CenterHefei 230031China School of Chemistry Physics and Mechanical EngineeringScience and Engineering FacultyQueensland University of TechnologyGardens Point CampusBrisbaneQLD 4001Australia

The thermodynamically favorable electrocatalytic oxidation coupled with hydrogen evolution reaction(HER)is considered as a sustainable and promising ***,it remains a great challenge due to the lack of simple,cheap,highefficient ***,we successfully develop a simple and scalable electro-deposition and subsequent phosphorization route to fabricate Ni-doped Co_(2)P(Ni-Co_(2)P)nanosheets catalyst using the in-situ released Ni species from defective Ni foam as metal ***,the as-synthesized Ni-Co_(2)P catalyst exhibits excellent electrochemical 5-hydroxymethylfurfural oxidation reaction(HOR)performance with>99%2,5-furandicarboxylic acid yield and>97%Faradaic efficiency at an ultralow potential of 1.29 V *** hydrogen electrode(RHE).Experimental characterization and theoretical calculation reveal that the atomically doped Ni species can enhance the adsorption of reactant and thus lower the reaction energy *** coupling the electrocatalytic HOR with HER,the employed two-electrode system using Ni-Co_(2)P and commercial Ni foam as anode and cathode,respectively,exhibits a low cell voltage of 1.53 V to drive a current density of 10 mA·cm^(−2),which is 90 mV lower than that of pure water *** work provides a facile and efficient approach for the preparation of high-performance earth-abundant electrocatalysts toward the concurrent production of H_(2)and value-added chemicals.

关键词： heteroatomic doping phosphide electrodes electrocatalytic oxidation hydrogen evolution reaction biomass conversion

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Promoting the electrochemical hydrogenation of furfural by synergistic Cu^(0)−Cu^(+) active sites

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Science China Chemistry 2022年第12期65卷 2588-2595页

作者： Zhongcheng Xia Yingying Li Jingcheng Wu Yu-Cheng Huang Weixing Zhao Yuxuan Lu Yuping Pan Xu Yue Yanjing Wang Chung-Li Dong Shuangyin Wang Yuqin Zou State Key Laboratory of Chem/Bio-Sensing and Chemometrics College of Chemistry and Chemical EngineeringAdvanced Catalytic Engineering Research Center of the Ministry of EducationHunan UniversityChangsha410082China Research Center for X-ray Science&Department of Physics Tamkang UniversityNew Taipei City25137China School of Chemistry and Chemical Engineering Jishou UniversityJishou416000China

Electrochemical hydrogenation(ECH)of furfural,which uses the proton from water and avoids the usage of gaseous hydrogen and high pressure,is an efficient way to utilize biomass ***-based catalysts are promising catalysts for the ECH of ***,their active sites and reaction mechanism have not been fully understood *** work unveils the active oxidation state of Cu-based electrocatalysts for the ECH of *** co-existence of Cu^(+)and Cu^(0) on the CuO surface under the working potential is confirmed by a series of in situ *** poisoning experiment shows that the performance decreased heavily after the Cu^(+)was complexed with SCN−,indicating the decisive role of Cu^(+).Finally,the density functional theory(DFT)calculation suggests that the Cu^(0)−Cu^(+)synergistic effect is beneficial to both kinetics and thermodynamics:Cu^(+)accelerates the second step hydrogenation process of furfural,and Cu^(0) reduces the energy barrier for the desorption of furfuryl *** work demonstrates the synergistic effect of Cu^(0) and Cu^(+)states for the electrochemical hydrogenation of furfural and provides a deeper understanding of the furfural hydrogenation mechanism.

关键词： biomass conversion electrocatalytic hydrogenation furfural CuO synergistic effect

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