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Relationship between hydrogenation degree and pyrolysis performance of jet fuel

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Chinese Journal of chemical engineering 2024年第4期68卷 35-42页

作者： Qing Liu Tinghao Jia Lun Pan Jijun Zou Xiangwen Zhang key laboratory for Green chemical and Technology School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China Haihe laboratory of Sustainable chemical Transformations Tianjin 300192China Zhejiang Institute of Tianjin University Ningbo 315201China Zhejiang provincial key laboratory of Advanced chemical engineering manufacture Technology College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027China

Understanding the relationship between the chemical composition and pyrolysis performance of endothermic hydrocarbon fuel(EHF)is of great significance for the design and optimization of advanced EHFs.In this work,the effect of deep hydrogenation on the pyrolysis of commercial RP-3 is investigated.Fuels with different hydrogenation degrees were obtained by the partially and completely catalytic hydrogenation and their pyrolysis performances were investigated using an apparatus equipped with an electrically heated tubular reactor.The results show that with the increase of hydrogenation degree,fuel conversion almost remains constant during the pyrolysis process(500e650C,4 MPa);however,the heat sink increases slightly,and the anti-coking performance significantly improves,which are highly related to their H/C ratios.Detailed characterisations reveal that the difference of the pyrolysis performance can be ascribed to the content of aromatics and cycloalkanes:the former are prone to initiate secondary reactions to form coking precursors,while the latter could act as the hydrogen donor and release hydrogen,which will terminate the radical propagation reactions and suppress the coke deposition.This work should provide the guidance for upgrading EHFs by modulating the composition of EHFs.

关键词： RP-3 Fuel Pyrolysis Hydrogenation Deposition

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Nano-alumina@cellulose-coated separators with the reinforcedconcrete-like structure for high-safety lithium-ion batteries

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Chinese Journal of chemical engineering 2024年第4期68卷 83-93页

作者： Zhihao Yang Li Chen Jian Xue Miaomiao Su Fangdan Zhang Liangxin Ding Suqing Wang Haihui Wang Guangdong provincial key lab of Green chemical Product Technology School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou 510640China Beijing key laboratory of Membrane Materials and engineering Department of Chemical EngineeringTsinghua UniversityBeijing 100084China

Separators play a critical role in the safety and performance of lithium-ion batteries.However,commercial polyolefin separators are limited by their poor affinity with electrolytes and low melting points.In this work,we constructed a reinforced-concrete-like structure by homogeneously dispersing nano-Al_(2)O_(3)and cellulose on the separators to improve their stability and performance.In this reinforcedconcrete-like structure,the cellulose is a reinforcing mesh,and the nano-Al_(2)O_(3)acts as concrete to support the separator.After constructing the reinforced-concrete-like structure,the separators exhibit good stability even at 200C(thermal shrinkage of 0.3%),enhanced tensile strain(tensile stress of 133.4 MPa and tensile strains of 62%),and better electrolyte wettability(a contact angle of 6.5°).Combining these advantages,the cells with nano-Al_(2)O_(3)@cellulose-coated separators exhibit stable cycling performance and good rate performance.Therefore,the construction of the reinforced-concretelike structure is a promising technology to promote the application of lithium-ion batteries in extreme environments.

关键词： Alumina Nanomaterials Lithium-ion batteries Membranes Cellulose Reinforced-concrete-like structure

Methane activation by[LnO]^(+):the 4f orbital matters

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Science China Chemistry 2024年第1期67卷 330-335页

作者： Bowei Yuan Jingxiang Zou Mincheng Yu Shaodong Zhou College of chemical and Biological engineering Zhejiang Provincial Key Laboratory of Advanced Chemical Engineering Manufacture TechnologyZhejiang UniversityHangzhou 310027China Zhejiang provincial Innovation Center of Advanced chemicals Technology Institute of Zhejiang University–QuzhouQuzhou 324000China laboratory for Sciences and Technologies of Energy Materials of Fujian Province(IKKEM) Xiamen 361005China

Gas-phase reactions of[LnO]^(+)with methane have been studied by using inductively coupled plasma-mass spectrometer(ICP-MS)combined with quantum chemical calculations.Experiments indicate that the[LnO]^(+)(Ln=Sm-Lu)ions are able to activate methane to generate methyl radicals.In particular,[EuO]^(+)and[YbO]^(+)exhibit the highest reactivity.Interestingly,ab initio computations reveal a novel HAT process operating in the absence of a terminal oxygen radical,as mediated by[EuO]^(+)and[YbO]^(+).Such a process diverges from previous findings on the methane activation by metal oxide clusters,not only on the electronic pattern during the course of hydrogen transfer,but also on the important role that 4f electrons play.The associated electronic origins have been discussed,and the well-designed 4f electron occupation may turn to be a promising approach in constructing lanthanide involved catalysts.

关键词： lanthanide oxides methane activation 4f orbitals quantum chemical calculation ion-molecule reaction

Highly selective electrosynthesis of 3,4-dihydroisoquinoline accompanied with hydrogen production over three-dimensional hollow CoNi-based microarray electrocatalysts

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Nano Research 2024年第4期17卷 2509-2519页

作者： Yu Xin Liyu Chen Yingwei Li Kui Shen Guangdong provincial key lab for Green chemical Product Technology School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou 510640China State key laboratory of Pulp and Paper engineering School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou 510640China

Electrocatalytic oxidation reaction of biomass-based derivatives is an excellent candidate to replace water oxidation for obtaining both value-added products and hydrogen(H_(2)),but the exploration of competent electrocatalysts is still highly challenging.Herein,two new types of three-dimensional self-supported hollow microarrays containing CoNi layered double hydroxide(CoNi-LDH)and N-doped carbon nanosheets decorated with CoNi alloyed nanoparticles(CoNi-NC)on carbon cloth(CC)are prepared,which are further used as efficient electrocatalysts for tetrahydroisoquinoline(THIQ)electrooxidation and hydrogen evolution reaction(HER),respectively.We demonstrate that the Co-modulated electronic environment for Ni(II)/Ni(Ⅲ)redox-looping in CoNi-LDH is the main factor to boost the selectivity of 3,4-dihydroisoquinoline(DHIQ)for the indirect electrooxidation process of THIQ.Density functional theory(DFT)calculations reveal that the Ni(Ⅲ)/Co(Ⅲ)dual sites of CoNi-LDH exhibit enhanced adsorption for THIQ but poorer adsorption for DHIQ compared to pure Co(Ⅲ)or Ni(Ⅲ).Therefore,the Ni(Ⅲ)/Co(Ⅲ)dual sites can effectively inhibit the peroxidation of DHIQ to isoquinoline(IQ)over CoNi-LDH,thus improving the selectivity of DHIQ to nearly 100%,much higher than that of its pure Ni counterpart.Moreover,CC@CoNi-NC can deliver high HER activity with low overpotential(40 mV@10 mA·cm^(-2))and high exchange current density(3.08 mA·cm^(-2)).Impressively,the assembled flow-cell device with CC@CoNi-LDH anode and CC@CoNi-NC cathode only requires low cell voltage and electricity consumption of 1.6 V and 3.50 kWh per cubic meter of H_(2)(@25 mA·cm^(-2)).

关键词： highly selective electrosynthesis dihydroisoquinolines hydrogen evolution reaction metal-organic frameworks hollow microarrays

Recycling of waste aluminum scraps to fabricate sulfidated zero-valent iron-aluminum particles for enhanced chromate removal

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Journal of Environmental Sciences 2024年第4期138卷 650-659页

作者： Yahui Zhang Liguo Zhang Jiajia Zeng Shuqun Xu Jianyu Pan Wenzhuo Huang Jianliang Sun Feng Jiang Guangdong provincial key laboratory of chemical Pollution and Environmental Safety&MOE key laboratory of Theoretical Chemistry of Environment School of EnvironmentSouth China Normal UniversityGuangzhou 510006China Guangdong provincial key lab of Environmental Pollution Control and Remediation Technology School of Environmental Science&EngineeringSun Yat-Sen UniversityGuangzhou 510275China

Massive waste aluminum scraps produced from the spent aluminum products have high electron capacity and can be recycled as an attractive alternative to materials based on zerovalent iron(Fe^(0))for the removal of oxidative contaminants from wastewater.This study thus proposed an approach to fabricate micron-sized sulfidated zero-valent iron-aluminum particles(S-Al^(0)@Fe^(0))with high reactivity,electron selectivity and capacity using recycled waste aluminum scraps.S-Al^(0)@Fe^(0)with a three-layer structure contained zero-valent aluminum(Al^(0))core,Fe^(0) middle layer and iron sulfide(FeS)shell.The rates of chromate(Cr(Ⅵ))removal by S-Al^(0)@Fe^(0)at pH 5.0-9.0 were 1.6-5.9 times greater than that by sulfidated zero-valent iron(S-Fe^(0)).The Cr(Ⅵ)removal capacity of S-Al^(0)@Fe^(0)was 8.2-,11.3-and 46.9-fold greater than those of S-Fe0,zero-valent iron-aluminum(Al^(0)-Fe^(0))and Fe^(0),respectively.The chemical cost of S-Al^(0)@Fe^(0) for the equivalent Cr(Ⅵ)removal was 78.5%lower than that of S-Fe^(0).Negligible release of soluble aluminum during the Cr(Ⅵ)removal was observed.The significant enhancement in the reactivity and capacity of S-Al^(0)@Fe^(0)was partially ascribed to the higher reactivity and electron density of the Al0core than Fe^(0).More importantly,S-Al^(0)@Fe^(0) served as an electric cell to harness the persistent and selective electron transfer from the Al^(0)-Fe^(0) core to Cr(Ⅵ)at the surface via coupling Fe^(0)-Fe^(2+)-Fe^(3+)redox cycles,resulting in a higher electron utilization efficiency.Therefore,S-Al^(0)@Fe^(0) fabricated using recycled waste aluminum scraps can be a cost-effective and environmentally-friendly alternative to S-Fe^(0) for the enhanced removal of oxidative contaminants in industrial wastewater.

关键词： Recycled waste aluminum scraps Oxidative contaminants Cr(Ⅵ)reduction Sulfidated Al^(0)@Fe^(0)particle Electron transfer

Controllable surface reconstruction of copper foam for electrooxidation of benzyl alcohol integrated with pure hydrogen production

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SmartMat 2024年第1期5卷 147-157页

作者： Yingnan Han Chang Yu Hongling Huang Qianbing Wei Junting Dong Lin Chen Jieshan Qiu State key lab of Fine chemicals School of Chemical EngineeringLiaoning Key Lab for Energy Materials and Chemical EngineeringDalian University of TechnologyDalianChina State key laboratory of chemical Resource engineering College of Chemical EngineeringBeijing University of Chemical TechnologyBeijingChina

Electrocatalytic water splitting that is coupled with electrocatalytic chemical oxidation is considered as one of the promising methods for efficiently obtaining hydrogen energy and fine chemicals.Herein,we focus on an electrochemical redox activation strategy to rationally manipulate the microstructure and surface valence states of copper foam(CF)and boost the corresponding performance towards electrocatalytic benzyl alcohol oxidation(EBA),accompanied by the efficient hydrogen production.Correspondingly,the Cu(II)‐dominated species are gradually formed on the CF surface with the dissolution and redeposition of copper in the suitable potential range.The new species containing Cu2O,CuO,and Cu(OH)2 during surface reconstruction process of the CF were confirmed by multiple characterization techniques.After 220‐cycled activation(CF‐220),the activated CF achieves an increase of current density for EBA in anode from 9.5 for the original CF to 29.3 mmol/cm2,while the pure hydrogen yield increases threefold than that of the original CF at 1.5 VRHE.The produced new species can endow the CF‐220 with abundant acidity sites,which can enhance the adsorption toward Lewis‐basicity benzyl alcohol,confirmed by NH3‐temperature‐programmed desorption.In situ Raman result further reveals that the as‐produced CuO,Cu(OH)2,and Cu(OH)42−are the main active species toward the EBA process.

关键词： benzyl alcohol copper electrochemical oxidation Lewis acid surface reconstruction

A novel and promising engineering application of carbon dots:Enhancing the chloride binding performance of cement

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Chinese chemical Letters 2024年第6期35卷 409-416页

作者： Wu-Jian Long Yang Yu Chuang He Guangdong provincial key laboratory of Durability for Marine Civil engineering Key Lab of Coastal Urban Resilient InfrastructureMOECollege of Civil and Transportation EngineeringShenzhen UniversityShenzhen 518060China

Corrosion of reinforcement induced by chloride invasion is extensively considered as the dominating deterioration mechanism of reinforced concrete(RC)structures,leading to serious safety hazards and tremendous economic losses.However,it still lacks well dispersive and cost-efficient nanomaterials to improve the anti-chloride-corrosion ability of RC structures.Herein,specific carbon dots(CDs)with high dispersity and low cost are deliberately designed,successfully prepared by hydrothermal processing,and then firstly applied to immensely enhance chloride binding performance of cement,thereby contributing to suppressing the corrosion of reinforcement.Specifically,the tailored CDs are composed of the carbon core with highly crystalline sp^(2)C structures and oxygen-containing groups connecting on the carbon core;The typical equilibrium test confirms that with respect to that of the blank cement paste,the chloride binding capacity of cement paste involving 0.2 wt%(by weight of cement)CDs is increased by 109% after 14-day exposure to 3 mol/L Na Cl solution;according to comprehensive analyses of phase compositions,the chloride binding mechanism of CDs-modified cement is rationally attributed to the fact that the incorporation of CDs advances the formation of calcium silicate hydrate(C-S-H)gels and Friedel's salt(Fs),thus enormously enhancing the physically adsorbed and chemically bound chloride ions of cement pastes.This work not only firstly provides a novel high-dispersity and low-cost nanomaterial toward the durability enhancement of RC structures,but also broadens the application of CDs in the field of engineering,conducing to stimulating their industrialization development.

关键词： Carbon dots Chloride binding Cement Chloride binding mechanism Friedel’s salt

Self-supported NiFe-LDH nanosheets on NiMo-based nanorods as high-performance bifunctional electrocatalysts for overall water splitting at industrial-level current densities

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Nano Research 2024年第5期17卷 3769-3776页

作者： Yan Zhang Biao Feng MingLei Yan Zhen Shen Yiqun Chen Jingyi Tian Fengfei Xu Guanghai Chen Xizhang Wang Lijun Yang Qiang Wu Zheng Hu key laboratory of Mesoscopic Chemistry of Ministry of Education(MOE)and Jiangsu provincial lab for Nanotechnology School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China College of Water Conservancy and Hydropower engineering Sichuan Agricultural UniversityYa’an 625014China

Efficient,durable and economic electrocatalysts are crucial for commercializing water electrolysis technology.Herein,we report an advanced bifunctional electrocatalyst for alkaline water splitting by growing NiFe-layered double hydroxide(NiFe-LDH)nanosheet arrays on the conductive NiMo-based nanorods deposited on Ni foam to form a three-dimensional(3D)architecture,which exhibits exceptional performances for both hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).In overall water splitting,only the low operation voltages of 1.45/1.61 V are required to reach the current density of 10/500 mA·cm^(-2),and the continuous water splitting at an industrial-level current density of 500 mA·cm^(-2) shows a negligible degradation(1.8%)of the cell voltage over 1000 h.The outstanding performance is ascribed to the synergism of the HER-active NiMo-based nanorods and the OER-active NiFe-LDH nanosheet arrays of the hybridized 3D architecture.Specifically,the dense NiFe-LDH nanosheet arrays enhance the local pH on cathode by retarding OH-diffusion and enlarge the electrochemically active surface area on anode,while the conductive NiMo-based nanorods on Ni foam much decrease the charge-transfer resistances of both electrodes.This study provides an efficient strategy to explore advanced bifunctional electrocatalysts for overall water splitting by rationally hybridizing HER-and OER-active components.

关键词： alkaline water splitting bifunctional electrocatalysts layered double hydroxides high durability industrial current densities

Enhancing Green Ammonia Electrosynthesis Through Tuning Sn Vacancies in Sn‑Based MXene/ MAX Hybrids

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Nano-Micro Letters 2024年第5期16卷 154-168页

作者： Xinyu Dai Zhen‑Yi Du Ying Sun Ping Chen Xiaoguang Duan Junjun Zhang Hui Li Yang Fu Baohua Jia Lei Zhang Wenhui Fang Jieshan Qiu Tianyi Ma key laboratory for Green Synthesis and Preparative Chemistry of Advanced Materials of Liaoning Province College of ChemistryInstitute of Clean Energy ChemistryLiaoning UniversityShenyang 110036People’s Republic of China State key laboratory of Clean and Efficient Coal Utilization Taiyuan University of TechnologyTaiyuan 030024People’s Republic of China School of Chemistry and chemical engineering Anhui UniversityHefei 230601People’s Republic of China School of chemical engineering The University of AdelaideAdelaideSA 5005Australia State key laboratory of High‑Efficiency Utilization of Coal and Green chemical engineering College of Chemistry and Chemical EngineeringNingxia UniversityYinchuan 750021NingxiaPeople’s Republic of China School of Science RMIT UniversityMelbourneVIC 3000Australia Guangdong provincial key laboratory of Advanced Energy Storage Materials School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou 510640People’s Republic of China College of chemical engineering State Key Laboratory of Chemical Resource EngineeringBeijing University of Chemical TechnologyBeijing 100029People’s Republic of China

Renewable energy driven N_(2) electroreduction with air as nitrogen source holds great promise for realizing scalable green ammonia production.However,relevant out-lab research is still in its infancy.Herein,a novel Sn-based MXene/MAX hybrid with abundant Sn vacancies,Sn@Ti_(2)CTX/Ti_(2)SnC–V,was synthesized by controlled etching Sn@Ti_(2)SnC MAX phase and demonstrated as an efficient electrocatalyst for electrocatalytic N2 reduction.Due to the synergistic effect of MXene/MAX heterostructure,the existence of Sn vacancies and the highly dispersed Sn active sites,the obtained Sn@Ti2CTX/Ti_(2)SnC–V exhibits an optimal NH_(3) yield of 28.4μg h^(−1) mg_(cat)^(−1) with an excellent FE of 15.57% at−0.4 V versus reversible hydrogen electrode in 0.1 M Na_(2)SO_(4),as well as an ultra-long durability.Noticeably,this catalyst represents a satisfactory NH3 yield rate of 10.53μg h^(−1) mg^(−1) in the home-made simulation device,where commercial electrochemical photovoltaic cell was employed as power source,air and ultrapure water as feed stock.The as-proposed strategy represents great potential toward ammonia production in terms of financial cost according to the systematic technical economic analysis.This work is of significance for large-scale green ammonia production.

关键词： Green ammonia synthesis N2 electroreduction Renewable energy Sn MXene/MAX hybrid