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Interfacial amine-assisted electrodeposition of superhydrophilic/superaerophobic metal hydroxides for robust oxygen evolution catalysis

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Science China Chemistry 2025年第5期68卷 2188-2195页

作者： Qing Chen keyu Wang Shiyi Li Yixing Wang Linfeng Lei Minghui Zhu Linzhou Zhuang Zhi Xu State Key Laboratory of Chemical Engineering School of Chemical EngineeringEast China University of Science and Technology Suzhou Laboratory

The oxygen evolution reaction（OER） is crucial for the electrocatalytic water electrolysis into oxygen and hydrogen,but the fourelectron transfer process hinders the OER *** realize the highly efficient water splitting,the nonprecious metal-based electrodes that can optimize the adsorption energy of intermediates and generate H2with low overpotential and robust stability are ***,we report a surface modification strategy to grow the trimetallic FeCoNi hydroxide on the amine linkersgrafted carbon cloth（CC-NH2@FeCoNi） by ***-NH2@FeCoNi possesses a superhydrophilic/superaerophobic surface,which could significantly enhance the mass transfer,and meanwhile promote the in situ generation of MOOH active ***,the superhydrophilic surface could facilitate the adsorption of abundant OH-ions,and repel the Cl-ions via electrostatic repulsive force during seawater ***,compared with the CC@FeCoNi that grown on the pure CC（320 mV）,the CC-NH2@FeCoNi needs an obviously smaller overpotential of 270 mV to achieve a current density of 100 mA cm-2,and meanwhile it exhibits a superior durability for 100 h at a current density of 200 m A cm-2in both alkaline water and *** strategy could be even applied universally in the preparation of other nonprecious metal hydroxides for efficient OER catalysis.

关键词： amine grafting superhydrophilicity superaerophobicity metal hydroxides water oxidation anticorrosion

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Insights into the role of oxygen-containing functional groups on carbon surface in water–electricity generation

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Nano Research 2024年第7期17卷 6645-6653页

作者： Wan Xue Zongbin Zhao Honghui Bi Bolun Zhang Xuzhen Wang Jieshan Qiu State Key Laboratory of Fine Chemicals Liaoning Key Laboratory for Energy Materials and Chemical EngineeringSchool of Chemical EngineeringDalian University of TechnologyDalian 116024China State Key Laboratory of Fine Chemicals Liaoning Key Laboratory for Energy Materials and Chemical EngineeringSchool of ChemistryDalian University of TechnologyDalian 116024China State Key Laboratory of Chemical Resource Engineering College of Chemical EngineeringBeijing University of Chemical TechnologyBeijing 100029China

A deep understanding of the electricity generation mechanism from the interaction between water molecules and carbon material surfaces is attractive for next-generation water-based energy conversion and storage ***,an asymmetric generator was assembled based on functionalized carbon nanotubes films to investigate the relative contribution from various oxygen functional groups on carbon surface to the water-electrical *** and calculations demonstrate that the electricity mainly originates from the water molecule adsorption by carboxyl groups and dissociation of functional groups on carbon surface,which leads to the formation of electrical double layers at *** device allows the electricity generation with a variety of water sources,such as deionized water,tap water,as well as *** particular,the generator based on carboxyl carbon nanotubes can induce a voltage of over 200 mV spontaneously in natural seawater with the power density of about 0.11 mW·g^(−1).High voltages can be achieved easily through the series-connection strategy to power electronic products such as a liquid crystal *** work reveals the dominant role of carboxyl groups in carbon-based water–electricity conversion and is expected to offer inspiration for the preparation of carbon materials with high electrical performance.

关键词： electricity generation water adsorption dissociation carboxyl groups carbon nanotubes

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Solar-driven salt-free deposition evaporation for simultaneous desalination and electricity generation based on tip-effect and siphon-effect

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Journal of Energy Chemistry 2024年第11期98卷 364-373页

作者： Wan Xue Zongbin Zhao Guanyu Zhao Honghui Bi Huijun Zhu Xuzhen Wang Jieshan Qiu State Key Laboratory of Fine Chemicals Liaoning Key Laboratory for Energy Materials and Chemical EngineeringSchool of Chemical EngineeringDalian University of TechnologyDalian 116024LiaoningChina State Key Laboratory of Fine Chemicals Liaoning Key Laboratory for Energy Materials and Chemical EngineeringSchool of ChemistryDalian University of TechnologyDalian 116024LiaoningChina State Key Laboratory of Chemical Resource Engineering College of Chemical EngineeringBeijing University of Chemical TechnologyBeijing 100029China

Solar-driven desalination is a promising way to alleviate the freshwater shortage,while is facing challenges posed by low evaporation rates and severe salt ***,a high-performance twodimensional(2D) solar absorber with Co_(3)O_(4) nanoneedle arrays(Co_(3)O_(4)-NN) grown on the surface of reduced graphene oxide-coated pyrolyzed silk cloth(Co_(3)O_(4)-NN/rGO/PSC) was prepared,and a salt-free evaporator system was assembled based on the composite material and siphonage-the flowing water *** is revealed that the evaporation enthalpy of water can be reduced over the 2D solar absorber grown with Co_(3)O_(4)-NN_T enabling an evaporation rate of up to 2.35 kg m^(-2) h^(-1) in DI water under one solar *** desalination process can be carried out continuously even with salt concentration up to 20 wt%,due to the timely removal of concentrated brine from the interface with the assistance of directed flowing ***,the 2D structure and the flowing water also provide an opportunity to convert waste solar heat into electricity in the evaporator based on the seebeck effect,ensuring simultaneous freshwater production and power *** is believed that this work provides insights into designing hybrid systems with high evaporation rate,salt resistance,and electricity generation.

关键词： Co_(3)O_(4)nanoneedle arrays Solar water evaporation Evaporation enthalpy Salt free Siphon effect Power generation

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Heterogeneously catalyzed self-condensation of n-butanal

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Chinese Journal of chemical engineering 2025年第4期80卷 89-99页

作者： Yaqi Qu Hualiang An Xinqiang Zhao Yanji Wang Hebei Provincial Key Laboratory of Green Chemical Technology and Efficient Energy Saving Tianjin Key Laboratory of Chemical Process SafetySchool of Chemical Engineering and TechnologyHebei University of TechnologyTianjin 300130China

The self-condensation of n-butanal is an important reaction for carbon-chain extension in the commercial production of ***,aldol condensation is one of the important reactions for the synthesis of valuable organic chemicals or transportation fuels from biomass-derived platform *** the investigation of the self-condensation of n-butanal is of significance in both academia and *** contribution reviewed the catalytic performance of heterogeneous catalysts in the self-condensation of n-butanal and the related reaction mechanism,network,and *** purpose of this review is to dedicate some help for further development of environmentally friendly catalysts and for a thorough comprehension of aldol condensation.

关键词： Aldol condensation n-Butanal Solid catalyst Reaction mechanism Reaction network Reaction kinetics

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Hydrophobic CHA-ZIFs with a junctional trap between cha and d6r cages for adsorption of 2,3-butanediol in aqueous solution

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Chinese Journal of chemical engineering 2024年第9期73卷 90-100页

作者： Lifang Ge Meizhen Gao Xiaosheng Zhang Jiang Wang Qi Shi Jinxiang Dong College of Chemical Engineering and Technology Shanxi Key Laboratory of Chemical Product EngineeringTaiyuan University of TechnologyTaiyuan 030024China

The adsorption and separation of diols from dilute aqueous solution using hydrophobic materials is very challenging due to the strong diol-water hydrogen-bonding interactions. Herein, we screened hydrophobic zeolitic imidazolate frameworks(ZIFs) with chabazite(CHA) topology for separation of 2,3-butanediol(2,3-BDO) and 1,3-propanediol(1,3-PDO), which had junctional and hydrophobic traps matching the two end methyl groups of the 2,3-BDO molecule. Based on CHA-ZIFs with the same small-sized ligand 2-methylimidazole(mIm) and different large-sized ligand benzimidazole derivatives(RbIm),CHA-ZIFs with larger surface areas were obtained by the addition of excess small-sized ligand mIm in the synthesis process. We showed that all of the hydrophobic CHA-ZIFs preferentially adsorbed 2,3-BDO over 1,3-PDO by static batch adsorption and dynamic column adsorption experiments. But ZIF-301 and ZIF-300 with halogen groups exhibited better adsorptive separation performance for 2,3-BDO/1,3-PDO than ZIF-302 with methyl groups. For a typical ZIF-301, its adsorption capacity for 2,3-BDO was 116.4 mg·g^(-1)and selectivity for 2,3-BDO/1,3-PDO was 3.8 in dynamic column adsorption of the binary-component system(2,3-BDO/1,3-PDO: 50 g·L^(-1)/50 g·L^(-1)). Computational simulations revealed that 2,3-BDO preferentially adsorbed in a trap at the junction between the cha and d6r cages of CHA-ZIFs,meaning the strong host-guest interactions. Therefore, the hydrophobic CHA-ZIFs with a junctional trap were promising candidate materials for adsorbing 2,3-BDO, which also provided a new perspective for separating diols in dilute aqueous solutions.

关键词： Adsorption Separation Aqueous solution Zeolitic imidazolate frameworks Junctional and hydrophobic trap Diols

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Effect of introducing oxygen into ethylene tar pitches on their carbonaceous products

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Chinese Journal of chemical engineering 2024年第12期76卷 135-146页

作者： Rongqi Chen Yongzheng Zhang Yanli Wang Chunyin Shen Liang Zhan Licheng Ling State Key Laboratory of Green Chemical Engineering and Industrial Catalysis Key Laboratory of Specially Functional Polymeric Materials and Related Technology(Ministry of Education)Shanghai Key Laboratory of Multiphase Materials Chemical EngineeringState Key Laboratory of Chemical EngineeringEast China University of Science and TechnologyShanghai 200237China

Ethylene tar is a prospective precursor for preparing carbonaceous materials,which is regarded as a representative soft carbon material after ***,the introduction of oxygen can influence the morphology of the final carbonaceous *** the introduction of oxygen,dealkylation and dehydrogenation will be promoted and the molecules can be linked more *** the subsequent carbonization,the biphenyl structures caused by the deoxygenation via the elimination of CO_(2),as well as the reserved aromatic ether bonds,can facilitate the strong cross-linking,which will restrain the movement of the carbon layers and the formation of the graphitic *** the graphitization treatment at 2800℃,the oxidized pitch can lead to short-range ordered and long-range unordered structures,while the sample without oxidation can result in long-range ordered graphitic *** can be proved that a simple oxidation-carbonization treatment can transform ethylene tar into hard carbon structures.

关键词： Fuel Oxidation Ethylene tar pitch Carbonization Hard carbon chemical processes

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Process intensification for the synthesis and purification of battery-grade Li_(2)CO_(3)with microfluidics

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Particuology 2024年第7期90卷 106-117页

作者： Haodu Li Jie Zhang Lin Dai Le Du Jiqin Zhu The State Key Laboratory of Chemical Resource Engineering College of Chemical EngineeringBeijing University of Chemical TechnologyBeijing 100029China

Battery-grade lithium carbonate(Li_(2)CO_(3))with a purity of higher than 99.5 wt%is of great importance as a high value-added lithium ***,influences of different reaction systems and process control on product purity remain ***,a membrane dispersion microreactor was used to enhance the mass transfer of preparation and purification processes in homogeneous and heterogeneous *** systems of Na_(2)CO_(3)–LiCl,NH_(4)HCO_(3)–LiCl,and NH_(3)·H_(2)O−CO_(2)−LiCl,CO_(2)purification based on carbonation and decomposition were *** Li_(2)CO_(3)purity was increased by the improvement of mixing *** carbonation time was reduced by 62.5%and 58.3%for the NH_(3)·H_(2)O−CO_(2)and CO_(2)purification systems,*** the two ammonia-based systems,Li_(2)CO_(3)particles with a purity of 99.7–99.8 wt%were one-step prepared with a size of 3–5μm,which also met the requirement of the battery-grade *** purity was further increased to 99.9 wt%by CO_(2)purification and LiHCO_(3)*** investigation could provide a feasible alternative for the controllable preparation of battery-grade Li_(2)CO_(3)in one or multiple steps.

关键词： Microfluidics Battery grade Li_(2)CO_(3) Process intensification High purity

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Ionic liquid-assisted preparation of hydroxyapatite and its catalytic performance for decarboxylation of itaconic acid

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Chinese Journal of chemical engineering 2024年第3期67卷 9-15页

作者： Shutong Pang Hualiang An Xinqiang Zhao Yanji Wang Hebei Provincial Key Laboratory of Green Chemical Technology and Efficient Energy Saving Tianjin Key Laboratory of Chemical Process SafetySchool of Chemical Engineering and TechnologyHebei University of TechnologyTianjin 300130China

The synthesis of methacrylic acid from biomass-derived itaconic acid is a green route,for it can get rid of the dependence on fossil *** order to solve the problems on this route such as use of a preciousmetal catalyst and a corrosive homogeneous alkali,we prepared a series of hydroxyapatite catalysts by an ionic liquid-assisted hydrothermal method and evaluated their catalytic *** results showed that the ionic liquid[Bmim]BF_(4) can affect the crystal growth of hydroxyapatite,provide fluoride ion for fluorination of hydroxyapatite,and adjust the surface acidity and basicity,morphology,textural properties,crystallinity,and composition of ***[Bmim]BF4 dosage and hydrothermal temperature can affect the fluoride ion concentration in the hydrothermal system,thus changing the degree of fluoridation of *** fluoride-ion concentration can lead to the formation of CaF_(2) and thus significantly decrease the catalytic performance of *** hydrothermal time mainly affects the growth of hydroxyapatite crystals on the c axis,leading to different catalytic *** suitable conditions for the preparation of this fluoridized hydroxyapatite are as follows:a mass ratio of[Bmim]BF4 to calcium salt=0.2:1,a hydrothermal time of 12 h,and a hydrothermal temperature of 130℃.A maximal methacrylic acid yield of 54.7%was obtained using the fluoridized hydroxyapatite under relatively mild reaction conditions(250℃ and 2 MPa of N_(2))in the absence of a precious-metal catalyst and a corrosive homogeneous alkali.

关键词： Ionic liquid Hydroxyapatite Itaconic acid Methacrylic Decarboxylation reaction

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Multivariate synergy for heightening ionic HOF robustness and proton conductivity

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Science China Chemistry 2025年第5期68卷 1879-1887页

作者： Xiang-Tian Bai Li-Hui Cao Xu-Yong Chen Jia-Yu Wang Zi-Ye Zhou Shaanxi Key Laboratory of Chemical Additives for Industry College of Chemistry and Chemical EngineeringShaanxi University of Science and Technology

Multicomponent crystalline materials construct more complex and diversified structures with different combinations and modes,which expands the material structure space and application fields. In this work, we have successfully synthesized two twocomponent ionic hydrogen-bonded organic frameworks（iHOF-32 and iHOF-33） and a three-component iHOF（iHOF-34）. Guanidine hydrochloride which is rich in N and H and has a short chain length strengthens the hydrogen bonding network of iHOF, thereby aiding in the efficient migration of protons. The rigid architecture of 1,1'-diamino-4,4'-bipyridine diiodide furnishes additional scaffolding for the iHOFs and enhances its robustness under harsh conditions. iHOF-34 accomplishes the combination of the ultra-high proton conductivity of iHOF-32 and the robustness of iHOF-33 by the synergistic interaction among the three components of ligands. In addition, iHOF-34 was fabricated as a composite membrane with a peak proton conductivity of 1.55 × 10-1S cm-1, which is 3.8 times higher than that of recast Nafion, and has extensive potential in fuel *** self-assembly strategy of multicomponent HOFs opens up new avenues for constructing diverse structures while promising new opportunities for applications in the fields of proton conduction and energy storage.

关键词： multivariate synergy ionic hydrogen-bonded organic framework robustness proton conduction

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Selective hydrogenation of dimethyl toluene-2,4-dicarbamate over supported Rh-based catalysts:Effect of support properties

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Chinese Journal of chemical engineering 2024年第11期75卷 102-109页

作者： Yaqi Qu Xiang Li Hualiang An Xinqiang Zhao Yanji Wang Hebei Provincial Key Laboratory of Green Chemical Technology and Efficient Energy Saving Tianjin Key Laboratory of Chemical Process SafetySchool of Chemical Engineering and TechnologyHebei University of TechnologyTianjin 300130China

The selective hydrogenation of dimethyl toluene-2,4-dicarbamate(TDC)to methyl cyclohexyl-2,4-dicarbamate(also called hydrogenated TDC,HTDC)is an essential process for non-phosgene synthesis of methylcyclohexane-2,***,we prepared a series of supported Rh-based catalysts by the excessive impregnation method and investigated their catalytic performance for the selective hydrogenation of *** emphasis was put on the influence of support properties on the catalytic *** the prepared catalysts,Rh/g-Al_(2)O_(3)performed the best:a HTDC yield of 88.4%was achieved with a 100%conversion of TDC under the conditions of 100℃,3 MPa and 1 ***,Rh/γ-Al_(2)O_(3)could be repetitively used for 4 times without a significant loss of its catalytic ***,XRD,N_(2)adsorption-desorption,H_(2)-TPR,NH_(3)/CO_(2)-TPD,XPS and ICP characterizations were employed to distinguish the properties of the prepared catalysts and the results were correlated with their catalytic *** is indicated that the yield of HTDC shows a positive relevance with the percentage of moderate-to-strong acid sites and the content of Rh^(n+)(n≥3)in the *** values of the percentage and the content can promote a strong interaction between Rh nanoparticles and the supports,facilitating both the transfer of electrons from Rh to the support and the formation of Rh^(n+)*** is conducive to activating the benzene ring of TDC and thereby improving the yield of HTDC.

关键词： Dimethyl toluene-2,4-dicarbamate Methyl cyclohexyl-2,4-dicarbamate Benzene ring hydrogenation Supported Rh-based catalysts Support properties

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