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Chinese Journal of chemical engineering 2024年第4期68卷 231-240页

作者： Peng Jiang Hao Zhang Guanhan Zhao Lin Li Tuo Ji Liwen Mu Xiaohua Lu Jiahua Zhu state key laboratory of materials-oriented chemical engineering College of Chemical EngineeringNanjing Tech UniversityNanjing 211816China

In the carbonate industry,deep decarbonization strategies are necessary to effectively remediate CO_(2).These strategies mainly include both sustainable energy supplies and the conversion of CO_(2)in downstream processes.This study developed a coupled process of biomass chemical looping H2 production and reductive calcination of CaCO_(3).Firstly,a mass and energy balance of the coupled process was established in Aspen Plus.Following this,process optimization and energy integration were implemented to provide optimized operation conditions.Lastly,a life cycle assessment was carried out to assess the carbon footprint of the coupled process.Results reveal that the decomposition temperature of CaCO_(3)in an H_(2)atmosphere can be reduced to 780℃(generally around 900℃),and the conversion of CO_(2)from CaCO_(3)decomposition reached 81.33%with an H2:CO ratio of 2.49 in gaseous products.By optimizing systemic energy through heat integration,an energy efficiency of 86.30%was achieved.Additionally,the carbon footprint analysis revealed that the process with energy integration had a low global warming potential(GWP)of-2.624 kg·kg^(-1)(CO_(2)/CaO).Conclusively,this work performed a systematic analysis of introducing biomass-derived H_(2)into CaCO_(3)calcination and demonstrated the positive role of reductive calcination using green H_(2)in mitigating CO_(2)emissions within the carbonate industry.

关键词： Biomass CaCO_(3)reductive calcination chemical looping Hydrogen production Carbon footprint Thermodynamics process

Recent progress on nanomaterial-based electrochemical dissolved oxygen sensors

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Chinese Journal of chemical engineering 2024年第4期68卷 103-119页

作者： Shaoqi Zhang Tao Liu Zhenyu Chu Wanqin Jin state key laboratory of materials-oriented chemical engineering College of Chemical EngineeringNanjing Tech UniversityNanjing 211816China

Dissolved oxygen(DO)usually refers to the amount of oxygen dissolved in water.In the environment,medicine,and fermentation industries,the DO level needs to be accurate and capable of online monitoring to guide the precise control of water quality,clinical treatment,and microbial metabolism.Compared with other analytical methods,the electrochemical strategy is superior in its fast response,low cost,high sensitivity,and portable device.However,an electrochemical DO sensor faces a trade-off between sensitivity and long-term stability,which strongly limits its practical applications.To solve this problem,various advanced nanomaterials have been proposed to promote detection performance owing to their excellent electrocatalysis,conductivity,and chemical stability.Therefore,in this review,we focus on the recent progress of advanced nanomaterial-based electrochemical DO sensors.Through the comparison of the working principles on the main analysis techniques toward DO,the advantages of the electrochemical method are discussed.Emphasis is placed on recently developed nanomaterials that exhibit special characteristics,including nanostructures and preparation routes,to benefit DO determination.Specifically,we also introduce some interesting research on the configuration design of the electrode and device,which is rarely introduced.Then,the different requirements of the electrochemical DO sensors in different application fields are included to provide brief guidance on the selection of appropriate nanomaterials.Finally,the main challenges are evaluated to propose future development prospects and detection strategies for nanomaterial-based electrochemical sensors.

关键词： Nanomaterial Dissolved oxygen Electrochemical sensor Nanostructures Detection principles

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Amorphous hybrid tungsten oxide–nickel hydroxide nanosheets used as a highly efficient electrocatalyst for hydrogen evolution reaction

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Nano Research 2024年第4期17卷 2499-2508页

作者： Chao Lyu Chenghai Dai Yiwei Tan state key laboratory of materials-oriented chemical engineering School of Chemistry and Chemical EngineeringNanjing Tech UniversityNanjing 211816China

There are more challenges for alkaline hydrogen evolution reaction(HER)via simultaneously expediting the electron-coupled water dissociation process(Volmer step)and the following electrochemical H_(2) desorption(Heyrovsky step).Hybrid amorphous electrocatalysts are highly desirable for efficient hydrogen evolution from water-alkali electrolyzers due to the bifunctionality for the different elementary steps of HER and optimal interactions with water molecules and the reactive hydrogen intermediates(Had).Herein,the synthesis of amorphous hybrid ultrathin(tungsten oxide/nickel hydroxide)hydrate(a-[WO_(3)/Ni(OH)_(2)]·0.2H_(2)O)nanosheets on nickel foam(NF)for efficient alkaline HER is described.The structural and composition features of a-[WO_(3)/Ni(OH)_(2)]·0.2H_(2)O are characterized in detailed.The resulting a-[WO_(3)/Ni(OH)_(2)]·0.2H_(2)O/NF electrocatalyst with the synergistic effect of both hybrid components for the HER elementary steps shows greatly improved the activity and durability for the HER with a low overpotential of-41 and-163 mV at-10 and-500 mA·cm^(-2),respectively,a Tafel slope as low as-72.9 mV·dec^(-1),and long-term stability of continuous electrolysis for at least 150 h accompanying by inappreciable overpotential change in 1 M KOH.In the hybrid a-[WO_(3)/Ni(OH)_(2)]·0.2H_(2)O,Ni(OH)_(2) and WO_(3) moieties are separately responsible for accelerating dissociative adsorption of water and weakening Had adsorption strength,which is beneficial to the improvement of the alkaline HER activity.

关键词： amorphous nanomaterial bimetallic electrocatalyst tungsten oxide ultrathin nanosheet hydrogen evolution reaction

Hollow ZIF-67-derived Co@N-doped carbon nanotubes boosting the hydrogenation of phenolic compounds to alcohols

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Chinese Journal of chemical engineering 2024年第2期66卷 157-166页

作者： Zhihao Guo Jiuxuan Zhang Lanlan Chen Chaoqun Fan Hong Jiang Rizhi Chen state key laboratory of materials-oriented chemical engineering Nanjing Tech UniversityNanjing 211816China

The selective hydrogenation of highly toxic phenolic compounds to generate alcohols with thermal stability,environmental friendliness,and non-toxicity is of great importance.Herein,a series of Co-based catalysts,named Co@NCNTs,were designed and constructed by direct pyrolysis of hollow ZIF-67(HZIF-67)under H_(2)/Ar atmosphere.The evolution of the catalyst surface from the shell layer assembled by ZIF-67-derived particles to the in situ-grown hollow nitrogen-doped carbon nanotubes(NCNTs)with certain length and density is achieved by adjusting the pyrolysis atmosphere and temperature.Due to the synergistic effects of in situ-formed hollow NCNTs,well-dispersed Co nanoparticles,and intact carbon matrix,the as-prepared Co@NCNTs-0.10-450 catalyst exhibits superior catalytic performance in the hydrogenation of phenolic compounds to alcohols.The turnover frequency value of Co@NCNTs-0.10-450is 3.52 h^(-1),5.9 times higher than that of Co@NCNTs-0.40-450 and 4.5 times higher than that of Co@NCNTs-0.10-550,exceeding most previously reported non-noble metal catalysts.Our findings provide new insights into the development of non-precious metal,efficient,and cost-effective metal-organic framework-derived catalysts for the hydrogenation of phenolic compounds to alcohols.

关键词： Phenolic compounds Hollow ZIF-67 pyrolysis Nitrogen-doped carbon nanotubes Reduction Multiphase reaction Catalysis

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Towards carbon neutrality of calcium carbide-based acetylene production with sustainable biomass resources

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Green Energy & Environment 2024年第6期9卷 1068-1078页

作者： Peng Jiang Guanhan Zhao Hao Zhang Tuo Ji Liwen Mu Xiaohua Lu Jiahua Zhu state key laboratory of materials-oriented chemical engineering College of Chemical EngineeringNanjing Tech UniversityNanjing211816China

Acetylene is produced from the reaction between calcium carbide(CaC_(2))and water,while the production of CaC_(2) generates significant amount of carbon dioxide not only because it is an energy-intensive process but also the raw material for CaC_(2) synthesis is from coal.Here,a comprehensive biomass-to-acetylene process was constructed that integrated several units including biomass pyrolysis,oxygen-thermal CaC_(2) fabrication and calcium looping.For comparison,a coal-to-acetylene process was also established by using coal as feedstock.The carbon efficiency,energy efficiency and environmental impacts of the bio-based calcium carbide acetylene(BCCA)and coal-based calcium carbide acetylene(CCCA)processes were systematically analyzed.Moreover,the environmental impacts were further evaluated by applying thermal integration at system level and energy substitution in CaC_(2) furnace.Even though the BCCA process showed lower carbon efficiency and energy efficiency than that of the CCCA process,life cycle assessment demonstrated the BCCA(1.873 kgCO_(2eq) kg-prod^(-1))a lower carbon footprint process which is 0.366 kgCO_(2eq) kg-prod^(-1) lower compared to the CCCA process.With sustainable energy(biomass power)substitution in CaC_(2) furnace,an even lower GWP value of 1.377 kgCO_(2eq) kg-prod^(-1) can be achieved in BCCA process.This work performed a systematic analysis on integrating biomass into industrial acetylene production,and revealed the positive role of biomass as raw material(carbon)and energy supplier.

关键词： Biomass pyrolysis CO_(2)mitigation Calcium carbide Acetylene Calcium loop

engineering particles towards 3D supraballs-based passive cooling via grafting CDs onto colloidal photonic crystals

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Chinese chemical Letters 2024年第4期35卷 457-463页

作者： Jie Wu Xiaoqing Yu Guoxing Li Su Chen state key laboratory of materials-oriented chemical engineering College of Chemical EngineeringNanjing Tech UniversityNanjing 210009China

Particle engineering has opened the floodgates to material science in both fundamental and application field. However, covalent interactions have not yet been adequately designed in the particle engineering for functional colloidal photonic crystals(CPCs). Herein, we achieved covalent coupling between carboxylrich poly(styrene-acrylic acid)(P(St-AA)) monodispersed colloidal particles and amine-rich carbon dots(CDs) based on an feasible and universal particle engineering strategy. The designed CDs-grafted P(St-AA)monodispersed colloidal particles initiate a hydrogen bond-driven assembly mode and ensure the construction of large-scale crack-free CPCs. Moreover, the CDs equipped with selective broad-band absorption capacity could improve the saturation of structural colors for high-visibility CPCs. Furthermore, an injectable photonic hydrogel(IPH) is developed to design CPC supraball hydrogel via integrating the CDsgrafted P(St-AA) CPC supraballs with supramolecular hydrogel. Combining superior flexibility, sufficient self-healing capacity of supramolecular hydrogel with visual optical information of our CPC supraballs, a cyclically reversible coding and decoding system was developed. Meanwhile, we firstly demonstrated the novel strategy of 3D supraballs-based passive cooling. The designed 3D CPC supraball hydrogel presents nearly full observation angle reflections behavior and excellent water evaporation capacity and achieves3.6 ℃ temperature drops, showing the application advantages in 3D thermal management. This work not only provides a new insight for manipulating optical properties of CPCs, but also demonstrates an easyto-perform platform, as well as indicates the direction for the promising application of CPCs.

关键词： Particle engineering Carbon dots Colloidal photonic crystals Passive cooling Digital coding

Facile synthesis of high-brightness green-emitting carbon dots with narrow bandwidth towards backlight display

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Chinese chemical Letters 2024年第5期35卷 277-282页

作者： Rui Cheng Tingting Zhang Xin Huang Jian Yu state key laboratory of materials-oriented chemical engineering College of Chemical EngineeringNanjing Tech UniversityNanjing 210009China

High-performance carbon dots(CDs)allowing the application in high-end display devices are highly desirable and usually limited by the absence of simple and easy synthesis methods.In this work,we exploited an easy-to-implement strategy for the one-step synthesis of green-emitting CDs(G-CDs)with superb optical properties.The G-CDs were synthesized using m-phenylenediamine(m-PD)as a single precursor,and the reaction reacted at 180℃for 12 h The resultant G-CDs exhibit high-purity and excitationindependent green fluorescence with the photoluminescence(PL)peak located at 516 nm,full width at half maximum(FWHM)of 46 nm,and PL quantum yield(QY)of∼80%under the 470nm excitation light.The G-CDs and corresponding composite film prepared with polyvinyl butyral(G-CDs@PVB)exhibit good PL stability after undergoing long-time storage for one year and 360 h exposure under 460nm blue light.The G-CDs@PVB film was used as color-conversion materials in green-emitting light-emitting diode(LED)application,exhibiting a Commission internationale de l’Eclairage(CIE)chromaticity coordinate of(0.21,0.44).The film was also used in CD-based liquid crystal display(CD-LCD)application,achieving a color gamut value of 85%.This work will offer a working basis for the synthesis of high-performance CDs as well as their application in displays.

关键词： Carbon dots One-step synthesis Narrow bandwidth High quantum yield Display

Easy-to-perform organic-solvent-free synthesis of carbon dots with strong green photoluminescence

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Chinese chemical Letters 2024年第3期35卷 373-378页

作者： Jiazhuang Guo Yifeng Chen Pan Zhang Ge Li Xiaoning Yang Cai-Feng Wang Su Chen state key laboratory of materials-oriented chemical engineering College of Chemical EngineeringNanjing Tech UniversityNanjing 210009China

Carbon dots(CDs)have been extensively studied owing to their fascinating optical properties and wide potential applications.Here,we report an easy-to-perform and organic-solvent-free synthesis strategy for green-emissive CDs(G-CDs)possessing high photoluminescence(PL)quantum yield(QY).The G-CDs are synthesized by heating the homogeneous precursors of citric acid and cyanamide in an open vessel,circumventing the use of organic solvents,complex operations,high-pressure reactors,and expensive instruments in the synthesis process.The effect of various reaction variables on the formation and the optical properties of G-CDs are systematically investigated.The resultant G-CDs show bright PL emission at 521 nm with PL QY up to 73%.Then a white light-emitting diode(LED)with Commission Internationable de L'Eclairage(CIE)coordinates of(0.33,0.34)and color rendering index(CRI)of 92 is constructed based on G-CDs/thermoplastic polyurethane(TPU)composite.Moreover,a visual microfluidic detection platform is designed by using G-CDs as fluorescent probes for rapid quantitative detection of Fe^(3+),Cu^(2+),and Mn^(2+)metal ions,which can realize synchronized testing of multiple samples.This study might promote the development and preparation methods of high-performance CDs with various optical applications.

关键词： Carbon dots Efficient synthesis Green fluorescence Quantum yield White LEDs Microfluidic detection platform

Low-energy-consumption temperature swing system for CO_(2) capture by combining passive radiative cooling and solar heating

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Green Energy & Environment 2024年第3期9卷 507-515页

作者： Ying-Xi Dang Peng Tan Bin Hu Chen Gu Xiao-Qin Liu Lin-Bing Sun state key laboratory of materials-oriented chemical engineering Jiangsu National Synergetic Innovation Center for Advanced Materials(SICAM)College of Chemical EngineeringNanjing Tech UniversityNanjing211816China

Temperature-swing adsorption(TSA)is an effective technique for CO_(2) capture,but the temperature swing procedure is energy-intensive.Herein,we report a low-energy-consumption system by combining passive radiative cooling and solar heating for the uptake of CO_(2) on commercial activated carbons(CACs).During adsorption,the adsorbents are coated with a layer of hierarchically porous poly(vinylidene fluoride-co-hexafluoropropene)[P(VdF-HFP)HP],which cools the adsorbents to a low temperature under sunlight through radiative cooling.For desorption,CACs with broad absorption of the solar spectrum are exposed to light irradiation for heating.The heating and cooling processes are completely driven by solar energy.Adsorption tests under mimicked sunlight using the CACs show that the performance of this system is comparable to that of the traditional ones.Furthermore,under real sunlight irradiation,the adsorption capacity of the CACs can be well maintained after multiple cycles.The present work may inspire the development of new temperature swing procedures with little energy consumption.

关键词： CO_(2)capture Solar heating Passive radiative cooling Temperature swing adsorption

Asymmetric copolyimide membranes fabricated by nonsolvent-induced phase separation for He/CH_(4) and He/N_(2) separation

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Frontiers of chemical Science and engineering 2024年第4期18卷 97-106页

作者： Ying Li Lu Wang Junyan Xie Yong Dai Xuehong Gu Xuerui Wang state key laboratory of materials-oriented chemical engineering College of Chemical EngineeringNanjing Tech UniversityNanjing 211816China Quzhou Membrane Material Innovation Institute Quzhou 324000China

Membrane gas separation is considered an energy-saving technique to extract He from natural gas due to no phase change and room temperature operation.However,the membrane performance was strongly limited by the trade-off between permeance and selectivity.Herein,novel 4,4′-(hexafluoroisopropylidene)diphthalic anhydride(6FDA)-2,2′-bis(3-amino-4-hydroxyphenyl)hexafluoropropane(APAF)-5-amino-2-(4-aminobenzene)benzimidazole(BIA)asymmetric membranes with a thickness of 300 nm were successfully prepared by the non-solvent induced phase separation method.The membrane performance was modulated by regulating dope solution compositions(e.g.,tetrahydrofuran and polymer concentration).The ideal He/CH_(4) selectivity was 124 and the optimized He permeance reached 87 GPU,beyond the current upper bound.He/CH_(4) selectivity was 75 and He permeance was 73 GPU for the binary mixture feed containing 0.2 mol%He.The membrane showed good resistance to CO_(2) and C_(2)H_(6),which are the typical impurities in natural gas.The 6FDA-APAF-BIA membranes have good stability(>160 h),which can provide great potential in He extraction from natural gas.

关键词： He separation membrane natural gas copolyimide