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Sequential pyrolysis for understanding specific influence of cellulose- and lignin-derived volatiles on properties of counterpart char

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Green Chemical Engineering 2024年第2期5卷 222-235页

作者： Yuewen Shao Chao Li Mengjiao Fan Guoming Gao Stelgen Inkoua Lijun Zhang Shu Zhang Jun Xiang Song Hu Xun Hu School of Material Science and Engineering University of JinanJinan250022China joint international research laboratory of biomass energy and materials College of Materials Science and EngineeringNanjing Forestry UniversityNanjing210037China State Key laboratory of Coal Combustion Huazhong University of Science and Technology430074China

Interactions of cellulose-and lignin-derived intermediates have been well documented during pyrolysis of lignocellulosic biomass.The reaction network for the interactions is rather complex,as cellulose-derived volatiles could interact/react with not only lignin-derived volatiles but also lignin-derived char and vice versa.To probe specifically the impacts of cellulose-derived volatiles on the lignin-derived char or the opposite,herein the sequential pyrolysis was performed by arranging cellulose in the upper bed with lignin in the lower bed or lignin above with cellulose below at 350 and 650℃,respectively.The results indicated that the sequential pyrolysis of cellulose→lignin or lignin→cellulose at 350℃induced increased char yield from formation of carbonaceous deposits via volatiles-char interactions.Compared with the lignin-derived volatiles,the cellulose-derived volatiles,especially aldehyde fractions,were more reactive towards the lignin-derived char at 350℃,forming oxygen-rich lignin-derived char with a higher yield,an abundance of aliphatic structures and consequently lower thermal stability.In sequential pyrolysis of lignin→cellulose,more aromatics-rich species were deposited on cellulose-derived char,but the lignin-derived volatiles were less reactive for enhancing the char yield.At 650℃,instead of polymerisation of the volatiles on the char,either the cellulose-or lignin-derived char catalyzed the cracking of the counterpart volatiles to remove the aliphatic functionalities,which made the char more aromatic and thermally more stable.

关键词： Cellulose Lignin Sequential pyrolysis Char Interaction

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Mg-Al-hydrotalcite with alkaline sites protects Ni/KIT-6 from formation of amorphous coke in glycerol steam reforming via tailoring reaction intermediates

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Frontiers of Chemical Science and Engineering 2024年第4期18卷 25-39页

作者： Yunyu Guo Yiran Wang Yuewen Shao Shu Zhang Yi Wang Song Hu Jun Xiang Xun Hu School of Material Science and Engineering University of JinanJinan 250022China joint international research laboratory of biomass energy and materials College of Materials Science and EngineeringNanjing Forestry UniversityNanjing 210037China State Key laboratory of Coal Combustion Huazhong University of Science and TechnologyWuhan 430074China

During steam reforming,the performance of a catalyst and amount/property of coke are closely related to reaction intermediates reaching surface of a catalyst.Herein,modification of reaction intermediates by placing Mg-Al-hydrotalcite above Ni/KIT-6 catalyst in steam reforming of glycerol was conducted at 300 to 600°C.The results revealed that the catalytic activity of Ni/KIT-6 in the lower bed was enhanced with either Mg1-Al5-hydrotalcite(containing more acidic sites)or Mg5-Al1-hydrotalcite(containing more alkaline sites)as upper-layer catalyst.The in situ infrared characterization of steam reforming demonstrated that Mg-Al-hydrotalcite catalyzed the deoxygenation of glycerol,facilitating the reforming of the partially deoxygenated intermediates over Ni/KIT-6.Mg-Al-hydrotalcite as protective catalyst,however,did not protect the Ni/KIT-6 from formation of more coke.Nonetheless,this did not lead to further deactivation of Ni/KIT-6 while Mg5-Al1-hydrotalcite even substantially enhanced the catalytic stability,even though the coke was much more significant than that in the use of single Ni/KIT-6(52.7%vs.28.6%).The reason beneath this was change of the property of coke from more aliphatic to more aromatic.Mg5-Al1-hydrotalcite catalyzed dehydration of glycerol,producing dominantly reaction intermediates bearing C=C,which formed the catalytic coke of with carbon nanotube as the main form with smooth outer walls as well as higher aromaticity,C/H ratio,crystallinity,crystal carbon size,thermal stability,and resistivity toward oxidation on Ni/KIT-6 in the lower bed.In comparison,the abundance of acidic sites on Mg1-Al5-hydrotalcite catalyzed the formation of more oxygen-containing species,leading to the formation of carbon nanotubes of rough surface on Ni/KIT-6.

关键词： steam reforming of glycerol Mg-Alhydrotalcite sacrificial catalyst reaction intermediates property of coke

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High-lattice-adapted surface modifying Na_(4)MnV(PO_(4))_(3) for better sodium storage

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Nano research 2024年第4期17卷 2728-2735页

作者： Chongran Song Shiyu Li Ying Bai international joint research laboratory of New energy materials and Devices of Henan Province School of Physics and ElectronicsAcademy for Advanced Interdisciplinary StudiesHenan UniversityKaifeng 475004China

Sodium-ion batteries(SIBs)are required to possess long cycle life when used for large-scale energy storage.The polyanionic Na_(4)MnV(PO_(4))_(3)(NMVP)reveals good cyclic stability due to its unique three-dimensional(3D)frame structure,but it still faces the challenge of interfacial degradation in practical applications.In this work,NASICON-type Na_(1.3)Al_(0.7)Ti_(1.3)(PO_(4))_(3)(NATP)was deposited on the surface of NMVP to promote interface stability by surface modification and gradient doping.As a result,the optimized NMVP@2%NATP released a capacity retention of 44.8%after 1000 cycles at 5 C,much higher than that of the initial NMVP(28.9%).The enhanced electrochemical performance was mainly attributed to NATP coating acting as a fast ion transport carrier and physical barrier,significantly facilitating the Na^(+)diffusion and isolating side reaction at the electrode/electrolyte interface.On the other hand,Ti_(4)^(+)and Al^(3+)cations from the NATP were partially doped inside the NMVP surface to boost the transport of Na^(+),and the perfect lattice matching of NVMP and NATP improved the interface and structural stability accompanying long cycling.This work demonstrated the effectiveness of surface modification with high lattice match material and provided new perspectives for high energy density solid-state SIBs.

关键词： high-lattice-adapted cathode surface modification sodium-ion batteries

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Surface iodine and pyrenyl-graphdiyne co-modified Bi catalysts for highly efficient CO_(2) electroreduction in acidic electrolyte

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Nano research 2024年第4期17卷 2381-2387页

作者： Min Zhang Juan Wang Xin Rong Xiu-Li Lu Tong-Bu Lu MOE international joint laboratory of materials Microstructure Institute for New Energy Materials and Low Carbon TechnologiesSchool of Materials Science and EngineeringTianjin University of TechnologyTianjin 300384China

CO_(2) electroreduction to formic acid/formate would contribute to alleviating the energy and climate crisis.This work reports a Bi-based catalyst derived from the in-situ electroreduction of Bi_(2)O_(2)CO_(3) modified with iodine and pyrenyl-graphdiyne(PGDY)on the surface for efficient electroreduction of CO_(2) in acidic electrolyte,with a high partial current density of 98.71 mA·cm^(-2) and high Faradaic efficiency(FE)>90%over the potential range from^(-1).2 to-1.5 V vs.reversible hydrogen electrode(RHE),as well as the long-term operational stability over 240 h without degradation in H-type cell.Experimental results and density function theory calculations show that the synergistic effect of surface iodine and PGDY is responsible for this active and extremely stable process of CO_(2) electroreduction via lowering the energy barriers for formation of*OCHO intermediate,suppressing the competitive HER by enhancing the concentration of both K+and CO_(2) at reaction interface,as well as preventing the dissolution and re-deposition of active Bi atoms on surface during catalytic reaction.This work provides new insight into designing highly active and stable electrocatalysts for CO_(2) reduction.

关键词： CO_(2) reduction electrocatalysis Bi-based catalysts acidic electrolyte

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Cobalt-based heterogeneous catalysts for photocatalytic carbon dioxide reduction

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Tungsten 2024年第2期6卷 410-421页

作者： Hong Yuan Jian-Hua Mei Yun-Nan Gong Di-Chang Zhong Tong-Bu Lu MOE international joint laboratory of materials Microstructure Institute for New Energy Materials and Low Carbon TechnologiesSchool of Materials Science and EngineeringTianjin University of TechnologyTianjin 300384China

Solar light-driven CO_(2)reduction to high value-added chemicals has considered as an outstanding way to solve energy crisis and climate warming.Recently,various photocatalysts have been developed to achieve this reaction.Among them,cobaltbased heterogeneous catalysts have attracted great interest because of their promising performance,product selectivity and stability.Herein,we systematically summarize the research progress of various cobalt-based heterogeneous catalysts for the photoreduction of CO_(2),such as single-atom cobalt,and cobalt-based oxides,nitrides,sulfi des,phosphides,metal-organic frameworks and covalent-organic frameworks.Meanwhile,the advantages and structure-activity relationship of these catalysts in photocatalytic CO_(2)reduction reaction are discussed.Finally,the challenges and prospects for constructing cobaltbased heterogeneous catalysts with high effi ciency are highlighted.

关键词： Cobalt Heterogeneous catalysts CO_(2)reduction Photocatalysis

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Thermal pretreatment of willow branches impacts yield and pore development of activated carbon in subsequent activation with ZnCl_(2) via modifying cellulose structure

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Chinese Journal of Chemical Engineering 2024年第5期69卷 227-237页

作者： Linghui Kong Chao Li Runxing Sun Shu Zhang Yi Wang Jun Xiang Song Hu Dong Wang Chuanjun Leng Xun Hu School of Material Science and Engineering University of JinanJinan 250022China joint international research laboratory of biomass energy and materials College of Materials Science and EngineeringNanjing Forestry UniversityNanjing 210037China State Key laboratory of Coal Combustion Huazhong University of Science and TechnologyWuhan 430074China Shandong BASAN Graphite New Material Plant Zibo 255311China

Development of pore structures of activated carbon(AC)from activation of biomass with ZnCl_(2) relies on content and structure of cellulose/hemicellulose in the feedstock.Thermal pretreatment of biomass could induce dehydration and/or aromatization to change the structure of cellulose/hemicellulose.This might interfere with evolution of structures of AC,which was investigated herein via thermal pretreatment of willow branch(WB)from 200 to 360℃and the subsequent activation with ZnCl_(2) at 550℃.The results showed that thermal pretreatment at 360℃(WB-360)could lead to substantial pyrolysis to form biochar,with a yield of 31.9%,accompanying with nearly complete destruction of cellulose crystals and remarkably enhanced aromatic degree.However,cellulose residual in WB-360 could still be activated to form AC-360 with specific surface area of 1837.9 m~2·g^(-1),which was lower than that in AC from activation of untreated WB(AC-blank,2077.8 m~2·g^(-1)).Nonetheless,the AC-200 from activation of WB-200 had more developed pores(2113.9 m~2·g^(-1))and superior capability for adsorption of phenol,due to increased permeability of ZnCl_(2) to the largely intact cellulose structure in WB-200.The thermal pretreatment did increase diameters of micropores of AC but reduced the overall yield of AC(26.8%for AC-blank versus 18.0%for AC-360),resulting from accelerated cracking but reduced intensity of condensation.In-situ infrared characterization of the activation showed that ZnCl_(2) mainly catalyzed dehydration,dehydrogenation,condensation,and aromatization but not cracking,suppressing the formation of derivatives of cellulose and lignin in bio-oil.The thermal pretreatment formed phenolic-OH and C=O with higher chemical innerness,which changed the reaction network in activation,shifting morphology of fibrous structures in AC-blank to“melting surface”in AC-200 or AC-280.

关键词： Thermal pretreatment Activation with ZnCl_(2) Willow branch Activated carbon Biochar

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Hollow Metal-Organic Framework/MXene/Nanocellulose Composite Films for Giga/Terahertz Electromagnetic Shielding and Photothermal Conversion

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Nano-Micro Letters 2024年第9期16卷 161-179页

作者： Tian Mai Lei Chen Pei‑Lin Wang Qi Liu Ming‑Guo Ma research Center of biomass Clean Utilization MOE Engineering Research Center of Forestry Biomass Materials and BioenergyBeijing Key Laboratory of Lignocellulosic ChemistryCollege of Materials Science and TechnologyBeijing Forestry UniversityBeijing 100083People’s Republic of China State Silica-Based materials laboratory of Anhui Province Bengbu 233000People’s Republic of China

With the continuous advancement of communication technology,the escalating demand for electromagnetic shielding interference(EMI)materials with multifunctional and wideband EMI performance has become urgent.Controlling the electrical and magnetic components and designing the EMI material structure have attracted extensive interest,but remain a huge challenge.Herein,we reported the alternating electromagnetic structure composite films composed of hollow metal-organic frameworks/layered MXene/nanocellulose(HMN)by alternating vacuum-assisted filtration process.The HMN composite films exhibit excellent EMI shielding effectiveness performance in the GHz frequency(66.8 dB at Kaband)and THz frequency(114.6 dB at 0.1-4.0 THz).Besides,the HMN composite films also exhibit a high reflection loss of 39.7 dB at 0.7 THz with an effective absorption bandwidth up to 2.1 THz.Moreover,HMN composite films show remarkable photothermal conversion performance,which can reach 104.6℃under 2.0 Sun and 235.4℃under 0.8 W cm^(−2),respectively.The unique micro-and macrostructural design structures will absorb more incident electromagnetic waves via interfacial polarization/multiple scattering and produce more heat energy via the local surface plasmon resonance effect.These features make the HMN composite film a promising candidate for advanced EMI devices for future 6G communication and the protection of electronic equipment in cold environments.

关键词： Metal-organic frameworks MXene Nanocellulose Electromagnetic shielding Photothermal conversion

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Engineering Strategies for Suppressing the Shuttle Effect in Lithium–Sulfur Batteries

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Nano-Micro Letters 2024年第1期16卷 187-221页

作者： Jiayi Li Li Gao Fengying Pan Cheng Gong Limeng Sun Hong Gao Jinqiang Zhang Yufei Zhao Guoxiu Wang Hao Liu joint international laboratory On Environmental and energy Frontier materials School of Environmental and Chemical EngineeringShanghai UniversityShanghaiPeople’s Republic of China Centre for Clean energy Technology University of Technology SydneyBroadwaySydneyNSW 2007Australia

Lithium–sulfur(Li–S)batteries are supposed to be one of the most potential next-generation batteries owing to their high theoretical capacity and low cost.Nevertheless,the shuttle effect of firm multi-step two-electron reaction between sulfur and lithium in liquid electrolyte makes the capacity much smaller than the theoretical value.Many methods were proposed for inhibiting the shuttle effect of polysulfide,improving corresponding redox kinetics and enhancing the integral performance of Li–S batteries.Here,we will comprehensively and systematically summarize the strategies for inhibiting the shuttle effect from all components of Li–S batteries.First,the electrochemical principles/mechanism and origin of the shuttle effect are described in detail.Moreover,the efficient strategies,including boosting the sulfur conversion rate of sulfur,confining sulfur or lithium polysulfides(LPS)within cathode host,confining LPS in the shield layer,and preventing LPS from contacting the anode,will be discussed to suppress the shuttle effect.Then,recent advances in inhibition of shuttle effect in cathode,electrolyte,separator,and anode with the aforementioned strategies have been summarized to direct the further design of efficient materials for Li–S batteries.Finally,we present prospects for inhibition of the LPS shuttle and potential development directions in Li–S batteries.

关键词： Shuttle effect Designed strategies Li-S battery Lithium polysulfides

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Steam reforming of acetic acid over Ni/biochar of low metal-loading:Involvement of biochar in tailoring reaction intermediates renders superior catalytic performance

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Chinese Journal of Chemical Engineering 2024年第4期68卷 241-252页

作者： Yunyu Guo Yiran Wang Shu Zhang Yi Wang Song Hu Jun Xiang Walid Nabgan Xun Hu School of Material Science and Engineering University of JinanJinan 250022China joint international research laboratory of biomass energy and materials College of Materials Science and EngineeringNanjing Forestry UniversityNanjing 210037China State Key laboratory of Coal Combustion Huazhong University of Science and TechnologyWuhan 430074China Departament d'Enginyeria Química Universitat Rovira i VirgiliTarragona 43007Spain

Biochar is a reactive carrier as it may be partially gasified with steam in steam reforming,which could influence the formation of reaction intermediates and modify catalytic behaviors.Herein,the Ni/biochar as well as two comparative catalysts,Ni/Al_(2)O_(3) and Ni/SiO_(2),with low nickel loading(2%(mass))was conducted to probe involvement of the varied carriers in the steam reforming.The results indicated that the Ni/biochar performed excellent catalytic activity than Ni/SiO_(2) and Ni/Al_(2)O_(3),as the biochar carrier facilitated quick conversion of the eOH from dissociation of steam to gasify the oxygen-rich carbonaceous intermediates like C]O and CeOeC,resulting in low coverage while high exposure of nickel species for maintaining the superior catalytic performance.In converse,strong adsorption of aliphatic intermediates over Ni/Al_(2)O_(3) and Ni/SiO_(2) induced serious coking with polymeric coke as the main type(21.5%and 32.1%,respectively),which was significantly higher than that over Ni/biochar(3.9%).The coke over Ni/biochar was mainly aromatic or catalytic type with nanotube morphology and high crystallinity.The high resistivity of Ni/biochar towards coking was due to the balance between formation of coke and gasification of coke and partially biochar with steam,which created developed mesopores in spent Ni/biochar while the coke blocked pores in Ni/Al_(2)O_(3) and Ni/SiO_(2) catalysts.

关键词： Steam reforming Acetic acid Ni/biochar catalyst Property of coke Reaction intermediates

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Importance of oxygen-containing functionalities and pore structures of biochar in catalyzing pyrolysis of homologous poplar

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Chinese Journal of Chemical Engineering 2024年第1期65卷 200-211页

作者： Li Qiu Chao Li Shu Zhang Shuang Wang Bin Li Zhenhua Cui Yonggui Tang Obid Tursunov Xun Hu School of Material Science and Engineering University of JinanJinan 250022China joint international research laboratory of biomass energy and materials College of Materials Science and EngineeringNanjing Forestry UniversityNanjing 210037China School of energy and Power Engineering Jiangsu UniversityZhenjiang 212013China Shandong BASAN Graphite New Material Plant Zibo 255311China Department of Power Supply and Renewable energy Sources National Research University TIIAMETashkent 100000Uzbekistan

Biochar and bio-oil are produced simultaneously in one pyrolysis process,and they inevitably contact and may interact,influencing the composition of bio-oil and modifying the structure of biochar.In this sense,biochar is an inherent catalyst for pyrolysis.In this study,in order to investigate the influence of functionalities and pore structures of biochar on its capability for catalyzing the conversion of homologous volatiles in bio-oil,three char catalysts(600C,800C,and 800AC)produced via pyrolysis of poplar wood at 600 or 800℃or activated at 800℃,were used for catalyzing pyrolysis of homologous poplar wood at 600℃,respectively.The results indicated that the 600C catalyst was more active than 800C and 800AC for catalyzing cracking of volatiles to form more gas(yield increase by 40.2%)and aromatization of volatiles to form more light or heavy phenolics,due to its abundant oxygen-containing functionalities acting as active sites.The developed pores of the 800AC showed no such catalytic effect but could trap some volatiles and allow their further conversion via sufficient aromatization.Nevertheless,the interaction with the volatiles consumed oxygen on 600C(decrease by 50%),enhancing the aromatic degree and increasing thermal stability.The dominance of deposition of carbonaceous material of a very aromatic nature over 800C and 800AC resulted in net weight gain and blocked micropores but formed additional macropores.The in situ diffuse reflectance infrared Fourier transform spectroscopy characterization of the catalytic pyrolysis indicated superior activity of 600C for removal of -OH,while conversion of the intermediates bearing C=O was enhanced over all the char catalysts.

关键词： Poplar wood Catalytic pyrolysis Char catalyst Volatile-char interaction Bio-oil

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