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Chinese Journal of chemical engineering 2024年第4期68卷 165-180页

作者： Xuexiang Fu Xing Tang Yi Xu Xintao Zhou Dengfeng Zhang faculty of chemical engineering Kunming University of Science and TechnologyKunming 650500China

In order to comprehend the applicability of microwave irradiation for recovering coalbed methane,it is necessary to evaluate the microwave irradiation-induced alterations in coals with varying levels of *** this work,the carbon molecular sieve combined with KMnO_(4)oxidation was selected to fabricate carbon molecular sieve with diverse oxidation degrees,which can serve as model substances toward ***,the microwave irradiation dependences of pores,functional groups,and highpressure methane adsorption characteristics of model substances were *** results indicated that microwave irradiation causes rearrangement of oxygen-containing functional groups,which could block the micropores with a size of 0.40-0.60 nm in carbon molecular sieve;meanwhile,naphthalene and phenanthrene generated by macro-molecular structure pyrolysis due to microwave irradiation could block the micropores with a size of 0.70-0.90 *** alterations in micropore structure weaken the saturated methane adsorption capacity of oxidized carbon molecular sieve by 2.91%-23.28%,suggesting that microwave irradiation could promote methane ***,the increased mesopores found for oxidized carbon molecular sieve after microwave irradiation could benefit CH4 *** summary,the oxidized carbon molecular sieve can act as model substances toward coals with different ***,microwave irradiation is a promising technology to enhance coalbed methane recovery.

关键词： Microwave irradiation Physicochemical property Coal matrix Adsorption Carbon molecular sieve

Deep eutectic solvents:Green multi-task agents for sustainable super green hydrogen technologies

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Journal of Energy Chemistry 2024年第5期92卷 357-382页

作者： Raiyan Al-Farsi Maan Hayyan Renewable Energy engineering Program Faculty of Engineering and TechnologyMuscat UniversityMuscat 130Oman chemical engineering Program Faculty of Engineering and TechnologyMuscat UniversityMuscat 130Oman

While reliance on renewable energy resources has become a reality, there is still a need to deploy greener and more sustainable methods in order to achieve sustainable development goals. Indeed, green hydrogen is currently believed to be a reliable solution for global warming and the pollution challenges arising from fossil fuels, making it the resilient fuel of the future. However, the sustainability of green hydrogen technologies is yet to be achieved. In this context, generation of green hydrogen with the aid of deep eutectic solvents(DESs) as green mixtures has been demonstrated as a promising research area. This systematic review article covers green hydrogen generation through water splitting and biomass fermentation when DESs are utilized within the generation process. It also discusses the incorporation of DESs in fuel cell technologies. DESs can play a variety of roles such as solvent, electrolyte, or precursor;colloidal suspension and reaction medium;galvanic replacement, shape-controlling, decoration, or extractive agent;finally oxidant. These roles are relevant to several methods of green hydrogen generation, including electrocatalysis, photocatalysis, and fermentation. As such, it is of utmost importance to screen potential DES formulations and determine how they can function in and contribute throughout the green hydrogen mobility stages. The realization of super green hydrogen generation stands out as a pivotal milestone in our journey towards achieving a more sustainable form of development;DESs have great potential in making this milestone achievable. Overall, incorporating DESs in hydrogen generation constitutes a promising research area and offers potential scalability for green hydrogen production, storage,transport, and utilization.

关键词： Watersplitting Biohydrogen Super green hydrogen Electrocatalysis Photocatalysis Fuel cell Power-to-X

Phosphine-Catalyzed [4+3] Annulation Reaction of Indole Derivatives with MBH Carbonates:A Facile Access to Indole-1,2-fused 1,4-Diazepinones and Azepines

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Chinese Journal of Chemistry 2024年第3期42卷 271-275页

作者： Yannan Zhu Haoran Jiang Yi-Ning Wang faculty of Chemistry and chemical engineering Yancheng Institute of TechnologyYanchengJiangsu224051 China

A phosphine-catalyzed [4+3] annulation between dinucleophilic indole derivatives and Morita−Baylis−Hillman (MBH) carbonates was discovered by using the N1 and N4′/C4′ nucleophilicities of the indole precursors,in which indoles act as four atom synthons. This protocol provides an efficient and facile access to indole-1,2-fused 1,4-diazepinones and azepines in good to high yields in one step,which illustrates potential synthetic utilities in drug discovery.

关键词： Phosphine catalysis [4+3]Annulation Indole derivatives Nitrogen heterocycles Organocatalysis

Promoting electrocatalytic nitrogen reduction to ammonia via dopant boron on two-dimensional materials

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Rare Metals 2024年第10期43卷 5117-5125页

作者： Ya-Hui Cui Wen-Cheng Ouyang Ai-Jun Gao Chang-Yuan Yu Li-Peng Zhang State Key Laboratory of Organic-Inorganic Composites College of Chemical EngineeringBeijing University of Chemical Technology College of Materials Science and engineering Beijing University of Chemical Technology College of Life Science and technology Beijing University of Chemical Technology

Electrocatalytic nitrogen reduction reaction(NRR) is a key process for producing energy efficient and environment friendly ammonia. Boron-doped two-dimensional materials are highly promising as NRR ***, the interaction between doped boron and matrix materials on NRR catalytic performance is still unclear,which is limiting the development of catalysts containing boron for NRR. Here, NRR on different boron-doped twodimensional(2D) materials was explored by first principle theory. It is found that adsorption energy of intermediate*NNH(E*NNH) can be used as a descriptor to characterize the catalytic activity for NRR. Boron-adsorbed black phosphorus(B-BP) is demonstrated showing excellent NRR catalytic activity and suppressing hydrogen evolution reaction. It is disclosed that the excellent catalytic performance of boron-doped structures comes from a proper quantitatively electron transfer(0.8e) between nitrogen in*NNH and the active site boron atom. This work not only established a descriptor for NRR catalytic activity on B-doped 2D materials, but also screened out a potential NRR catalyst. More importantly, the intrinsic reason and mechanism of high catalytic activity of boron-doped structures were proposed. This work provides a design principle for exploring high-performance NRR electrocatalysts containing boron.

关键词： Boron-doped two-dimensional materials Density functional theory Descriptor Electrocatalytic nitrogen reduction reaction

Recovery of scandium from silicate minerals by high-pressure leaching in sulfuric acid

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Journal of Rare Earths 2024年第7期42卷 1375-1384,I0007页

作者： Peng Yan Xiaoming Chen Likun Gao Bo Yang faculty of Metallurgical and Energy engineering Kunming University of Science and TechnologyKunming650093China faculty of Land Resources engineering Kunming University of Science and TechnologyKunming650093China School of Chemistry and chemical engineering Kunming UniversityKunming650214China

This study investigated the leaching of scandium from a Sc-bearing silicate *** Sc concentrate obtained by beneficiation pre-enrichment has 1.03×10^(−4) wt%Sc and 14.66 wt%*** main Sc-bearing minerals are limonite,chlorite,sericite,and hornblende,in the form of ***-pressure leaching(HPL)with sulfuric acid(98 wt%)and NaF was used to dispose this *** Sc leaching efficiency of 91.82%was obtained under the optimum conditions,which are pressure of 5.0×10^(5) Pa,A/O value of 1.1,L/S value of 1.8,NaF dosage of 2 wt%,at 130℃ for 6 *** X-ray diffraction(XRD)and scanning electron microscopy(SEM)results show that the residue is mainly quartz phase in the multihole *** with ordinary leaching for silicate,high-pressure leaching has significant advantages in saving acid and energy consumption.

关键词： Silicate minerals Scandium High-pressure Leaching Concentrated sulfuric acid Rare earths

Improved length of calcium sulfate crystal seeds and whiskers via ball milling and hydration treatment

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Chinese Journal of chemical engineering 2024年第7期71卷 102-109页

作者： Yuke Li Yuxin Liu Jizhen Huang Yi Mei faculty of chemical engineering Kunming University of Science and TechnologyKunming 650500China Yunnan Provincial Key Laboratory of Energy Saving in Phosphorus chemical engineering and New Phosphorus Materials Kunming University of Science and TechnologyKunming 650500China

Elucidating the effect of growth periods on the quality of calcium sulfate whiskers(CSWs)prepared from calcium sulfate dihydrate(DH)is ***,crystal seeds and whiskers were prepared from DH in a water–glycerol *** whiskers were obtained from crystal seeds prepared via hydration of DH for 30 s than via ball milling for 5 min followed by hydration for 20 *** attachment of cetyltrimethyl ammonium bromide and glycerol additives to the whisker tops promoted whisker *** whisker sponges exhibited good thermal barrier properties and compression cycle stability.

关键词： Hemihydrate gypsum whisker Hydration Ball milling/hydration Crystal seed Growth process

High adsorption selectivity of activated carbon and carbon molecular sieve boosting CO_(2)/N_(2) and CH_(4)/N_(2) separation

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Chinese Journal of chemical engineering 2024年第3期67卷 282-297页

作者： Siang Chen Wenling Wu Zhaoyang Niu Deqi Kong Wenbin Li Zhongli Tang Donghui Zhang The Research Center of chemical engineering School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China

Flue gas and coal bed methane are two important sources of greenhouse *** swing adsorption process has a wide range of application in the field of gas separation,and the selection of adsorbent is *** this regard,in order to assess the better adsorbent for separating CO_(2) from flue gas and CH_(4) from coal bed methane,adsorption isotherms of CO_(2),CH_(4) and N_(2) on activated carbon and carbon molecular sieve are measured at 303.15,318.15 and 333.15 K,and up to 250 *** experimental data fit better with Langmuir 2 compared to Langmuir 3 and Langmuir-Freundlich models,and Clausius-Clapeyron equation was used to calculate the isosteric *** the order of the adsorbed amount and the adsorption heat on the two adsorbents are CO_(2)>CH_(4)>N_(2).The adsorption kinetics are calculated by the pseudo-first kinetic model,and the order of adsorption rates on activated carbon is N_(2)-CH_(4)>CO_(2),while on carbon molecular sieve,it is CO_(2)-N_(2)>CH_(4).It is shown that relative molecular mass and adsorption heat are the primary effect on kinetics for activated carbon,while kinetic diameter is the main resistance factor for carbon molecular ***,the adsorption selectivity of CH_(4)/N_(2) and CO_(2)/N_(2) were estimated with the ideal adsorption solution theory,and carbon molecular sieve performed best at 318.15 K for both CO_(2) and CH_(4) *** study suggested that activated carbon is a better choice for separating flue gas and carbon molecular sieve can be a strong candidate for separating coal bed methane.

关键词： Activated carbon Carbon molecular sieve Adsorbent evaluation Adsorption equilibrium and kinetics Heat of adsorption Selectivity

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

Effectively improving the extreme-pressure capacity of a class of intercalated zirconium phosphate materials

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Science China(Technological Sciences) 2024年第3期67卷 753-764页

作者： NIU WenXing ZHAO XinRui YUAN Min HOU ZhiGuo LIU Lei XU Hong DONG JinXiang Shanxi Key Laboratory of chemical Product engineering Cllege of Chemical Engineering and TechnologyTaiyuan University of TechnologyTaiyuan 030024China School of chemical and Environmental engineering Pingdingshan UniversityPingdingshan 467000China

We studied different long-chain ammonium ions intercalated zirconium phosphate α-ZrP, methylamine intercalated ZrP(MAZrP), tetramethylammonium hydroxide intercalated ZrP(TMAH-ZrP), dodecyltrimethylammonium bromide intercalated ZrP(DTAB-ZrP), and stearyl trimethyl ammonium bromide intercalated ZrP(STAB-ZrP) as grease co-additives in combination with isobutylene sulfide(SIB). The grease with co-additives displayed excellent extreme-pressure and anti-wear ***, the combination of the longest chain ammonium ion intercalated zirconium phosphate, STAB-ZrP/SIB, had the best tribological properties. In comparison to α-ZrP, the advantage of STAB-ZrP was that it did not form a large area of the dense physical film like α-ZrP on the worn surface, but rather gave the SIB a chance to contact with the fresh metal surface to generate a chemical film. Therefore, the sub-micron physical film and nanoscale chemical film always exist side by side on the contact surface during the friction process. This intercalated α-ZrP/SIB additive has great potential for use in harsh operating conditions.

关键词： intercalatedα-ZrP/SIB physical film chemical film tribological properties

NaBH4-induced phase transition of CoSe_(2) with abundant Se deficiency for acidic oxygen reduction to hydrogen peroxide

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Rare Metals 2024年第2期43卷 500-510页

作者： Cai-Di Han Yong-Chao Zhang Qian Zhang Jin-Ting Wu Jian Gao Ji-Jun Zou Xiao-Dong Zhu State Key Laboratory Base of Eco-chemical engineering College of chemical engineering Qingdao University of Science and TechnologyQingdao266042China Key Laboratory for Green chemical technology of Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin300072China

Electrocatalytic oxygen reduction(ORR)via the 2e−pathway to form H_(2)O_(2) in acidic medium has attracted extensive ***,the low activity,insufficient selectivity and high cost of catalysts have been the ***,CoSe_(2) with abundant Se deficiency was synthesized by a simple hydrothermal method,and the addition of NaBH4-induced CoSe_(2) phase transition from orthorhombic to cubic phase with more Se *** cubic phase CoSe_(2) with abundant Se deficiency can effectively regulate the surface electronic structure with suitable binding energies of*OOH and*O,which shows high activity,selectivity and long-term stability for acidic ORR to H_(2)O_(2).The onset potential is as low as 0.73 V *** hydrogen electrode(RHE),the H_(2)O_(2) selectivity is 84%(0 V ***),and the average electron transfer number is about ***,the H_(2)O_(2) yield measured using a flow cell is as high as 115.92 mmol·gcat.^(−1)·h^(−1) and the Faradaic efficiency is 70%at 0 V ***,which presents high potential in electrocatalytic acidic ORR to H_(2)O_(2) and organic pollutant degradation using the electron-Fenton process.

关键词： Se defected CoSe_(2) Crystal phase transition Electrocatalysis Acidic oxygen reduction Hydrogen peroxide