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Synergy of heterogeneous Co/Ni dual atoms enabling selective C-O bond scission of lignin coupling with in-situ N-functionalization

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Journal of Energy Chemistry 2024年第5期92卷 16-25页

作者： Baoyu Wang Jinshu Huang Hongguo Wu Ximing Yan Yuhe Liao Hu Li National key laboratory of green Pesticide Key Laboratory of Green Pesticide&Agricultural BioengineeringMinistry of EducationState-Local Joint Laboratory for Comprehensive Utilization of BiomassCollege of Pharmacy&Center for R&D of Fine ChemicalsGuizhou UniversityGuiyang 550025GuizhouChina Guangxi key laboratory of green chemical Materials and Safety Technology Beibu Gulf UniversityQinzhou 535011GuangxiChina Guangzhou Institute of Energy Conversion Chinese Academy of SciencesGuangzhou 510640GuangdongChina

Selective cleavage of Csp^(2)-OCH_(3)bond in lignin without breaking other types of C-O bonds followed by N-functionalization is fascinating for on-purpose valorization of biomass.Here,a Co/Ni-based dual-atom catalyst CoNiDA@NC prepared by in-situ evaporation and acid-etching of metal species from tailor-made metal–organic frameworks was efficient for reductive upgrading of various lignin-derived phenols to cyclohexanols(88.5%–99.9%yields),which had ca.4 times higher reaction rate than the single-atom catalyst and was superior to state-of-the-art heterogeneous catalysts.The synergistic catalysis of Co/Ni dual atoms facilitated both hydrogen dissociation and hydrogenolysis steps,and could optimize adsorption configuration of lignin-derived methoxylated phenols to further favor the Csp^(2)-OCH_(3)cleavage,as elaborated by theoretical calculations.Notably,the CoNi_(DA)@NC catalyst was highly recyclable,and exhibited excellent demethoxylation performance(77.1%yield)in real lignin monomer mixtures.Via in-situ cascade conversion processes assisted by dual-atom catalysis,various high-value N-containing chemicals,including caprolactams and cyclohexylamines,could be produced from lignin.

关键词： Biomass conversion Heterogeneous catalysis Lignin Dual-atom catalyst Selective C-ocleavage

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Slippery hydrogel with desiccation-tolerant‘skin’for high-precision additive manufacturing

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International Journal of Extreme Manufacturing 2024年第2期6卷 486-500页

作者： Desheng Liu Pan Jiang Yue Hu Yaozhong Lu Yixian Wang Jiayu Wu Danli Hu Tao Wu Xiaolong Wang state key laboratory of Solid Lubrication Lanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou 730000People’s Republic of China CAS key laboratory of Chemistry of Northwestern Plant Resources Lanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou 730000People’s Republic of China Shandong laboratory of Advanced Materials and green Manufacturing at Yantai Yantai Zhongke Research Institute of Advanced Materials and Green Chemical EngineeringYantai 264006People’s Republic of China key laboratory of Materials-Oriented chemical engineering of Xinjiang Uygur Autonomous Region School of Chemistry and Chemical EngineeringShihezi UniversityShihezi 832003People’s Republic of China

Hydrogels inevitably undergo dehydration,structural collapse,and shrinkage deformation due to the uninterrupted evaporation in the atmosphere,thereby losing their flexibility,slipperiness,and manufacturing precision.Here,we propose a novel bioinspired strategy to construct a spontaneously formed‘skin’on the slippery hydrogels by incorporating biological stress metabolites trehalose into the hydrogel network,which can generate robust hydrogen bonding interactions to restrain water evaporation.The contents of trehalose in hydrogel matrix can also regulate the desiccation-tolerance,mechanical properties,and lubricating performance of slippery hydrogels in a wide range.Combining vat photopolymerization three-dimensional printing and trehalose-modified slippery hydrogels enables to achieve the structural hydrogels with high resolution,shape fidelity,and sophisticated architectures,instead of structural collapse and shrinkage deformation caused by dehydration.And thus,this proposed functional hydrogel adapts to manufacture large-scale hydrogels with sophisticated architectures in a long-term process.As a proof-of-concept demonstration,a high-precision and sophisticated slippery hydrogel vascular phantom was easily fabricated to imitate guidewire intervention.Additionally,the proposed protocol is universally applicable to diverse types of hydrogel systems.This strategy opens up a versatile methodology to fabricate dry-resistant slippery hydrogel for functional structures and devices,expanding their high-precision processing and broad applications in the atmosphere.

关键词： slippery hydrogel trehalose desiccation tolerance vat photopolymerization 3D printing hydrogen bonding

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A Generic Strategy to Create Mechanically Interlocked Nanocomposite/Hydrogel Hybrid Electrodes for Epidermal Electronics

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Nano-Micro Letters 2024年第5期16卷 120-133页

作者： Qian Wang Yanyan Li Yong Lin Yuping Sun Chong Bai Haorun Guo Ting Fang Gaohua Hu Yanqing Lu Desheng Kong College of engineering and Applied Sciences National Laboratory of Solid State Microstructureand Collaborative Innovation Center of Advanced MicrostructuresNanjing UniversityNanjing 210023People’s Republic of China state key laboratory of Analytical Chemistry for Life Science and Jiangsu Key Laboratory of Artificial Functional MaterialsNanjing UniversityNanjing 210023People’s Republic of China College of chemical engineering and Technology Engineering Research Center of Seawater Utilization Technology of Ministry of EducationState Key Laboratory of Reliability and Intelligence of Electrical EquipmentHebei University of TechnologyTianjin 300130People’s Republic of China key laboratory of Intelligent Optical Sensing and Manipulation Nanjing UniversityNanjing 210093People’s Republic of China

Stretchable electronics are crucial enablers for next-generation wearables intimately integrated into the human body.As the primary compliant conductors used in these devices,metallic nanostructure/elastomer composites often struggle to form conformal contact with the textured skin.Hybrid electrodes have been consequently developed based on conductive nanocomposite and soft hydrogels to establish seamless skin-device interfaces.However,chemical modifications are typically needed for reliable bonding,which can alter their original properties.To overcome this limitation,this study presents a facile fabrication approach for mechanically interlocked nanocomposite/hydrogel hybrid electrodes.In this physical process,soft microfoams are thermally laminated on silver nanowire nanocomposites as a porous interface,which forms an interpenetrating network with the hydrogel.The microfoam-enabled bonding strategy is generally compatible with various polymers.The resulting interlocked hybrids have a 28-fold improved interfacial toughness compared to directly stacked hybrids.These electrodes achieve firm attachment to the skin and low contact impedance using tissue-adhesive hydrogels.They have been successfully integrated into an epidermal sleeve to distinguish hand gestures by sensing mus-cle contractions.Interlocked nanocomposite/hydrogel hybrids reported here offer a promising platform to combine the benefits of both materials for epidermal devices and systems.

关键词： Stretchable electronics Epidermal electronics Silver nanowire Conductive nanocomposites Hydrogel

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Selective hydrodeoxygenation of guaiacol to cyclohexanol using activated hydrochar-supported Ru catalysts

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Frontiers of chemical Science and engineering 2024年第5期18卷 13-22页

作者： Kaile Li Shijie Yu Qinghai Li Yanguo Zhang Hui Zhou key laboratory for Thermal Science and Power engineering of Ministry of Education Beijing Key Laboratory of CO2 Utilization and Reduction TechnologyDepartment of Energy and Power EngineeringTsinghua UniversityBeijing 100084China Department of chemical and Biomolecular engineering National University of SingaporeSingapore117585Singapore

Lignin,an abundant aromatic polymer in nature,has received significant attention for its potential in the production of bio-oils and chemicals owing to increased resource availability and environmental issues.The hydrodeoxygenation of guaiacol,a lignin-derived monomer,can produce cyclohexanol,a nylon precursor,in a carbon-negative and environmentally friendly manner.This study explored the porous properties and the effects of activation methods on the Ru-based catalyst supported by environmentally friendly and cost-effective hydrochar.highly selective cleavage of C_(ary)-O bonds was achieved under mild conditions(160°C,0.2 MPa H2,and 4 h),and alkali activation further improved the catalytic activity.Various characterization methods revealedthat hydrothermal treatment and alkali activation relatively contributed to the excellent performance of the catalysts and influenced their porous structure and Ru dispersion.X-ray photoelectron spectroscopy results revealed an increased formation of metallic ruthenium,indicating the effective regulation of interaction between active sites and supports.This synergistic approach used in this study,involving the valorization of cellulose-derived hydrochar and the selective production of nylon precursors from lignin-derived guaiacol,indicated the comprehensive and sustainable utilization of biomass resources.

关键词： hydrochar guaiacol cyclohexanol activation full-component utilization

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Construction of multifunctional lanthanum manganese mixed nanoparticles mediated by ionic liquids for selective aerobic oxidation of cyclohexane

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Rare Metals 2024年第5期43卷 2205-2221页

作者： Hao Li Rui-Rui Zhang Ke-Xin Li Shuang Wei Yu-Mei Liu Rui-Xia Liu Beijing key laboratory of Ionic Liquids Clean Process CAS Key Laboratory of Green Process and Engineering State Key Laboratory of Multiphase Complex Systems Institute of Process Engineering Chinese Academy of Sciences University of Chinese Academy of Sciences

Selective oxidation of alkanes to produce highvalue chemicals is an essential strategy and means to realize efficient utilization of resources.In this work,a strategy of lanthanum manganese mixed metal oxides(LMMO) regulated via a facile ionic liquid (IL)-assisted hydrothermal method was proposed to construct the multifunctional catalysts,which exhibited excellent catalytic performance in the selective aerobic oxidation of cyclohexane.An 8.9%cyclohexane conversion with 90%KA oi(cyclohexanol and cyclohexanone) selectivity was achieved over the optimal LMMO catalyst under mild conditions.The effects of anion type,carbon chain length and concentration of ILs on the structure and properties of catalysts were investigated through various characterizations,indicating the structure-directing and template effect of ILs on the multifunctional catalysts.The formation of self-assembled spherical nanoparticles followed the‘‘dissolution-nucleation-proliferation’’mechanism with the introduction of 1-butyl-3-methylimidazolium hydrogen sulfate,ascribing the synergistic effect between the microenvironment of ILs and the hydrothermal environment.Importantly,the high reactive oxygen concentration redox capacity,and suitable basic sites of LMMO catalysts mediated by ILs enhance the activation of C-H bonds and molecular oxygen,simultaneously influencing the adsorption and desorption of the substrate.A comprehensive understanding of the high KA oil selectivity and radical reaction mechanism was elucidated based on in situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS) and radical trapping experiments.The recycling and regeneration experiments further illuminated that the removal of adsorbed cyclohexanone acting on the LMMO catalyst was the key to achieve high KA oil selectivity.

关键词： Ionic liquids Nanoparticle Multifunctional catalyst Cyclohexane oxidation

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Thermodynamic theory of flotation for a complex multiphase solid -liquid system and high-entropy flotation

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International Journal of Minerals,Metallurgy and Materials 2024年第6期31卷 1177-1197页

作者： Shuming Wen state key laboratory of Complex Nonferrous Metal Resources Clean utilization Faculty of Land Resource EngineeringKunming University of Science and TechnologyKunming 650093China

The flotation of complex solid–liquid multiphase systems involve interactions among multiple components,the core problem facing flotation theory.Meanwhile,the combined use of multicomponent flotation reagents to improve mineral flotation has become an important issue in studies on the efficient use of refractory mineral resources.However,studying the flotation of complex solid–liquid systems is extremely difficult,and no systematic theory has been developed to date.In addition,the physical mechanism associated with combining reagents to improve the flotation effect has not been unified,which limits the development of flotation theory and the progress of flotation technology.In this study,we applied theoretical thermodynamics to a solid–liquid flotation system and used changes in the entropy and Gibbs free energy of the reagents adsorbed on the mineral surface to establish thermodynamic equilibrium equations that de-scribe interactions among various material components while also introducing adsorption equilibrium constants for the flotation reagents adsorbed on the mineral surface.The homogenization effect on the mineral surface in pulp solution was determined using the chemical potentials of the material components of the various mineral surfaces required to maintain balance.The flotation effect can be improved through synergy among multicomponent flotation reagents;its physical essence is the thermodynamic law that as the number of compon-ents of flotation reagents on the mineral surface increases,the surface adsorption entropy change increases,and the Gibbs free energy change of adsorption decreases.According to the results obtained using flotation thermodynamics theory,we established high-entropy flotation theory and a technical method in which increasing the types of flotation reagents adsorbed on the mineral surface,increasing the adsorption entropy change of the flotation reagents,decreasing the Gibbs free energy change,and improving the adsorption efficiency and stability of the flotation reagents improve

关键词： multicomponent flotation reagent adsorption entropy change equations of thermodynamic equilibrium adsorption equilibri-um constant high-entropy flotation

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Interfacial mechanism of hydrogel with controllable thickness for stable drag reduction

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Friction 2024年第2期12卷 231-244页

作者： Xiaotong WU Ying LIU Yunlei ZHANG Xingwei WANG Wufang YANG Lang JIANG Shuanhong MA Meirong CAI Feng ZHOU School of Advanced Manufacturing Nanchang UniversityNanchang 330031China state key laboratory of Solid Lubrication Lanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou 730000China Yantai Zhongke Research Institute of Advanced Materials and green chemical engineering Shandong Laboratory of Yantai Advanced Materials and Green ManufactureYantai 264006China

Surface wettability plays a significant role in reducing solid–liquid frictional resistance,especially the superhydrophilic/hydrophilic interface because of its excellent thermodynamic stability.In this work,poly(acrylic acid)-poly(acrylamide)(PAA–PAM)hydrogel coatings with different thicknesses were prepared in situ by polydopamine(PDA)-UV assisted surface catalytically initiated radical polymerization.Fluid drag reduction performance of hydrogel surface was measured using a rotational rheometer by the plate–plate mode.The experimental results showed that the average drag reduction of hydrogel surface could reach up to about 56%in Couette flow,which was mainly due to the interfacial polymerization phenomenon that enhanced the ability of hydration layer to delay the momentum dissipation between fluid layers and the diffusion behavior of surface.The proposed drag reduction mechanism of hydrogel surface was expected to shed new light on hydrogel–liquid interface interaction and provide a new way for the development of steady-state drag reduction methods.

关键词： steady state drag reduction hydrogel interface hydration hydrophilic

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Recent advances in the microfluidic generation of shape-controllable hydrogel microparticles and their applications

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green chemical engineering 2024年第1期5卷 16-30页

作者： Yingzhe Liu Zhuo Chen Jianhong Xu The state key Lab of chemical engineering Department of Chemical EngineeringTsinghua UniversityBeijing100084China

Hydrogel microparticles,generally accepted as significant green materials,have been widely used in chemical,biological,and biomedical fields owing to their excellent biocompatibility,biodegradability,and noncytotoxicity.Among these,non-spherical hydrogel microparticles with diverse shape anisotropy have great potential in applications such as drug delivery,cellular interaction,micromotors,etc.Benefiting from their shapes,their functionalities in such fields cannot be satisfied by the typical spherical types.Recently,microfluidics with precise control and domination of fluids at microflow sizes has emerged as a powerful method for synthesizing shape-controllable hydrogel microparticles with good monodispersity and unique morphology.In this review,we tried to provide an overview of the production of non-spherical microparticles composed of green hydrogel materials,emphasizing the microfluidic approaches.Furthermore,a brief introduction to their current applications is also presented.

关键词： Microfluidics Hydrogel Microparticles Non-spherical Anisotropic green materials

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Long‐life lithium batteries enabled by a pseudo‐oversaturated electrolyte

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Carbon Energy 2024年第4期6卷 115-127页

作者： Youchun Yu Simeng Wang Juyan Zhang Weiwei Qian Nana Zhang Guangjie Shao Haiyan Bian Yuwen Liu Lan Zhang Hebei key laboratory of Applied Chemistry College of Environmental and Chemical EngineeringYanshan UniversityQinhuangdaoChina Beijing key laboratory of Ionic Liquids Clean Process CAS Key Laboratory of Green Process and EngineeringInstitute of Process EngineeringChinese Academy of SciencesBeijingChina Haike Group Research Institute of Innovation&Technology DongyingChina Langfang green Industrial Technology Center LangfangChina

The specific energy of Li metal batteries(LMBs)can be improved by using high‐voltage cathode materials;however,achieving long‐term stable cycling performance in the corresponding system is particularly challenging for the liquid electrolyte.Herein,a novel pseudo‐oversaturated electrolyte(POSE)is prepared by introducing 1,1,2,2‐tetrafluoroethyl‐2,2,3,3‐tetrafluoropropyl ether(TTE)to adjust the coordination structure between diglyme(G2)and lithium bis(trifluoromethanesulfonyl)imide(LiTFSI).Surprisingly,although TTE shows little solubility to LiTFSI,the molar ratio between LiTFSI and G2 in the POSE can be increased to 1:1,which is much higher than that of the saturation state,1:2.8.Simulation and experimental results prove that TTE promotes closer contact of the G2 molecular with Li^(+)in the POSE.Moreover,it also participates in the formation of electrolyte/electrode interphases.The electrolyte shows outstanding compatibility with both the Li metal anode and typical high‐voltage cathodes.Li||Li symmetric cells show a long life of more than 2000 h at 1 mA cm^(−2),1 mAh cm^(−2).In the meantime,Li||LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)cell with the POSE shows a high reversible capacity of 134.8 mAh g^(−1 )after 900 cycles at 4.5 V,1 C rate.The concept of POSE can provide new insight into the Li^(+)solvation structure and in the design of advanced electrolytes for LMBs.

关键词： high voltage lithium metal batteries pseudo‐oversaturated electrolyte solid electrolyte interphases(SEI) solvation structure

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Decarboxylative Amination with Nitroarenes via Synergistic Catalysis

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Chinese Journal of Chemistry 2024年第4期42卷 351-355页

作者： Meiling Ding Sitian Zhou Shunruo Yao Chengjian Zhu Weipeng Li Jin Xie state key laboratory of Coordination Chemistry Jiangsu Key Laboratory of Advanced Organic MaterialsChemistry and Biomedicine Innovation Center(ChemBIC)School of Chemistry and Chemical EngineeringNanjing UniversityNanjingJiangsu210023 China green Catalysis Center and College of ChemistryZhengzhou UniversityZhengzhouHenan450001 China

In this paper,we have developed a decarboxylative amination of carboxylic acids with nitroarenes for the synthesis of secondary amines.The protocol is performed at mild conditions without the use of noble metals as catalysts.A wide range of structurally diverse secondary amines could be obtained in good yields(up to 94%)with good functional group tolerance.This transformation shows good to excellent selectivity,avoiding the generation of over alkylated byproducts.

关键词： Nitroarenes Amines Synergistic catalysis Carboxylic acids Radical alkylation Amination Photocatalysis Steric hindrance

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