Chinese Journal of Chemical Engineering最新文献

{"title":"Toward the rational design for low-temperature hydrogenation of silicon tetrachloride: Mechanism and data-driven interpretable descriptor","authors":"Zhe Ding ,&nbsp;Li Guo ,&nbsp;Fang Bai ,&nbsp;Chao Hua ,&nbsp;Ping Lu ,&nbsp;Jinyi Chen","doi":"10.1016/j.cjche.2024.10.032","DOIUrl":"10.1016/j.cjche.2024.10.032","url":null,"abstract":"<div><div>Low-temperature hydrogenation of silicon tetrachloride (STC) is an essential step in polysilicon production. The addition of CuCl to silicon powder is currently a commonly used catalytic method and the silicon powder acts as both a reactant and a catalyst. However, the reaction mechanism and the structure-activity relationship of this process have not been fully elucidated. In this work, a comprehensive study of the reaction mechanism in the presence of Si and Cu₃Si was carried out using density functional theory (DFT) combined with experiments, respectively. The results indicated that the rate-determining step (RDS) in the presence of Si is the phase transition of Si atom, meanwhile, the RDS in the presence of Cu₃Si is the TCS-generation process. The activation barrier of the latter is smaller, highlighting that the interaction of Si with the bulk phase is the pivotal factor influencing the catalytic activity. The feasibility of transition metal doping to facilitate this step was further investigated. The Si disengage energy (<em>E</em>_d) was used as a quantitative parameter to assess the catalytic activity of the catalysts, and the optimal descriptor was determined through interpretable machine learning. It was demonstrated that d-band center and electron transfer play a crucial role in regulating the level of <em>E</em>_d. This work reveals the mechanism and structure-activity relationship for the low-temperature hydrogenation reaction of STC, and provides a basis for the rational design of catalysts.</div></div>","PeriodicalId":9966,"journal":{"name":"Chinese Journal of Chemical Engineering","volume":"79 ","pages":"Pages 172-184"},"PeriodicalIF":3.7,"publicationDate":"2025-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143580114","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Research on application of salt-free reductants in uranium/neptunium/plutonium separation","authors":"Qi Chen,&nbsp;Tianchi Li,&nbsp;Ziqian Zhao,&nbsp;Yifu Hu,&nbsp;Baole Li,&nbsp;Taihong Yan,&nbsp;Guoan Ye","doi":"10.1016/j.cjche.2024.11.009","DOIUrl":"10.1016/j.cjche.2024.11.009","url":null,"abstract":"<div><div>In current spent nuclear fuel reprocessing, the predominant method involves chemical extraction, leveraging the differing distribution ratios of elements to achieve separation and purification. Effective separation of uranium (U), plutonium (Pu), and neptunium (Np) typically relies on redox processes that alter their oxidation states during extraction. Therefore, reductants play a critical role in reprocessing processes. An important shift in the advanced reprocessing process is the use of salt-free reagents in the actinide separation process. In addition, the salt content in the reprocessing stream is often indicative of the overall technological sophistication of the process, and it is critical to reform the reductants used in the main process stream. Salt-free reductants have attracted much attention in recent years for basic and applied research in reprocessing processes because of their advantages such as being easily destroyed, not introducing salts, reacting quickly, simplifying the process, and reducing the amount of waste. This study summarizes emerging salt-free reagents with potential applications in reprocessing, and outlines their kinetic and chemical reaction mechanism properties in reducing Pu(IV) and Np(VI). The conclusion discusses the future potential of salt-free reagents in reprocessing. This study summarizes the currently well-studied salt-free reductants and offers recommendations and future research directions in salt-free alternatives.</div></div>","PeriodicalId":9966,"journal":{"name":"Chinese Journal of Chemical Engineering","volume":"79 ","pages":"Pages 30-44"},"PeriodicalIF":3.7,"publicationDate":"2025-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143534020","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Evaporation crystallization for the extraction of potassium bromide from bitters by phase equilibrium","authors":"Yulong Zhang ,&nbsp;Yun Li ,&nbsp;Hongfei Guo ,&nbsp;Dong Xu ,&nbsp;Jilin Cao","doi":"10.1016/j.cjche.2024.11.015","DOIUrl":"10.1016/j.cjche.2024.11.015","url":null,"abstract":"<div><div>Aiming at the problems of complex process and high cost in the production of potassium bromide at present, the solubility data and the phase diagram of the quaternary system KBr–MgBr₂–K₂SO₄–MgSO₄–H₂O at 298.15 K were studied using the isothermal dissolution equilibrium method. The results showed that there are eight invariant points, sixteen univariant curves, and nine crystallization regions in the phase diagram which is complex and contains two double salts (K₂SO₄·MgSO₄·6H₂O and KBr·MgBr₂·6H₂O) and a metastable phase (MgSO₄·5H₂O). On the basis of the Pitzer model and HW model, the solubilities of the quaternary system were calculated, with which the corresponding phase diagram was plotted. By comparison, the evaluated phase diagram is in accordance with the measured one. Through analysis, the phase diagrams of the quaternary system at (298.15 and 323.15) K were combined to put forward a process to separate KBr from the system by evaporation and crystallization, which realized the full circulation of the mother solution.</div></div>","PeriodicalId":9966,"journal":{"name":"Chinese Journal of Chemical Engineering","volume":"79 ","pages":"Pages 212-218"},"PeriodicalIF":3.7,"publicationDate":"2025-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143580122","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Noncovalently functionalized organic graphene aerogel composite for high-performance proton storage","authors":"Jing He ,&nbsp;Maoding Cheng ,&nbsp;Qinglong Jiang ,&nbsp;Subramania Angaiah ,&nbsp;Minjie Shi ,&nbsp;Chao Yan","doi":"10.1016/j.cjche.2024.11.018","DOIUrl":"10.1016/j.cjche.2024.11.018","url":null,"abstract":"<div><div>Although organic compounds are considered to be promising electrode materials with their remarkable characteristics such as diverse structures, design controllability, and environmental friendliness, their low charge-transfer capability and limited cycling durability hinder their application in aqueous proton batteries. Herein, we prepared a noncovalent phenazine-based graphene aerogel (H/G) composite for aqueous proton storage, which is realized by redox-active Hexaazatrinaphthalene (HATN) organic compound combined with conductive reduced graphene oxide (rGO). The integration of rGO into HATN not only effectively optimizes the electronic structure of the H/G composite to enhance its electrochemical activity, but also the favorable noncovalent π–π interaction existed between HATN and rGO provides a stable structure for fast electron transportation. The obvious electron transfer in the aerogel composite promotes fast and reversible redox reactions occurred with the imino-active HATN in the composite electrode for proton uptake/removal in an aqueous acidic electrolyte, which are demonstrated by in-situ Fourier transform infrared (FTIR) investigation, theoretical calculations and experimental measurements. Therefore, it can deliver a fast, stable and efficient aqueous proton storage behavior with a large specific capacity of 274 mAh g⁻¹ and considerable calendar life with ∼100% capacity retention after 3000 cycles, surpassing previously reported proton-based organic electrodes in aqueous acidic electrolytes. Furthermore, an outstanding soft-package aqueous proton (APB) has been fabricated with considerable long-term cycling stability.</div></div>","PeriodicalId":9966,"journal":{"name":"Chinese Journal of Chemical Engineering","volume":"79 ","pages":"Pages 260-268"},"PeriodicalIF":3.7,"publicationDate":"2025-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143601161","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Investigation of the formation processes of CO2 hydrate films on the interface of liquid carbon dioxide with humic acids solutions","authors":"Aleksey K. Sagidullin ,&nbsp;Sergey S. Skiba ,&nbsp;Tatyana P. Adamova ,&nbsp;Andrey Y. Manakov","doi":"10.1016/j.cjche.2024.10.030","DOIUrl":"10.1016/j.cjche.2024.10.030","url":null,"abstract":"<div><div>Morphology and growth rate of carbon dioxide hydrate on the interface between liquid carbon dioxide and humic acid solutions were studied in this work. It was found that after the growth of the hydrate film at the interface, further growth of hydrate due to the suction of water in the capillary system formed between the wall of the cuvette and the end boundary of the hydrate layer occurs. Most probably, substantial effects on the formation of this capillary system may be caused by variations in reactor wall properties, for example, hydrophobic-hydrophilic balance, roughness, <em>etc.</em> We found, that the rate of CO₂ hydrate film growth on the surface of the humic acid aqueous solution is 4-fold to lower in comparison with the growth rate on the surface of pure water. We suppose that this is caused by the adsorption of humic acid associates on the surface of hydrate particles and, as a consequence, by the deceleration of the diffusion of dissolved carbon dioxide to the growing hydrate particle.</div></div>","PeriodicalId":9966,"journal":{"name":"Chinese Journal of Chemical Engineering","volume":"79 ","pages":"Pages 53-61"},"PeriodicalIF":3.7,"publicationDate":"2025-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143561973","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"In-situ construction of morphology-controllable flower-shaped lignin-derived carbon/ZnO composite for efficient photocatalytic degradation of organic dyes","authors":"Zhengtao Wei ,&nbsp;Xiaofei Wang ,&nbsp;Xuliang Lin ,&nbsp;Xueqing Qiu","doi":"10.1016/j.cjche.2024.11.010","DOIUrl":"10.1016/j.cjche.2024.11.010","url":null,"abstract":"<div><div>The emission of organic pollutants from the dye industry and medical treatment represents a significant threat to the quality of water resources and human health. The development of green, environmentally friendly and efficient photocatalysts for the removal of organic pollutants from the environment is of paramount importance in addressing these issues. Flower-like lignin-derived carbon (LC)/zinc oxide (ZnO) composites with controllable morphology were synthesized via a direct precipitation method. In this study, alkali lignin was employed as an anionic active agent to alter the molecular arrangement on the liquid surface during the synthesis reaction and to reduce the surface tension between mixtures, thereby forming a special stacked morphology, which was then used for the highly efficient removal of methylidene blue (MB) and tetracycline hydrochloride (TCH) in water under different light conditions. The formation mechanism of LC/ZnO and the degradation characteristics under different reaction conditions were investigated. The loading of LC can form composites with large specific surface area and rich porous structure. In addition, with the help of lignin, the morphology of ZnO was changed from a rod-like structure to a lamellar structure, and LC could effectively reduce the band gap of ZnO, which could improve the electron transfer rate in the photocatalytic process. The ·O₂⁻ and ·OH radicals generated under photoexcitation promoted the decomposition of pollutants. This study presents a simple, economical, and scalable method for the application of photocatalysts and explores new ways for the high-value application of industrial lignin.</div></div>","PeriodicalId":9966,"journal":{"name":"Chinese Journal of Chemical Engineering","volume":"79 ","pages":"Pages 241-251"},"PeriodicalIF":3.7,"publicationDate":"2025-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143580596","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Synthesis of a porous organic polymer via click reaction for efficient CH4/C2H6/C3H8 separation","authors":"Xun Wang,&nbsp;Tianjian Lun,&nbsp;Changbin Xu,&nbsp;Haolong Zheng,&nbsp;Daofei Lv,&nbsp;Xin Chen,&nbsp;Jian Yan,&nbsp;Junjie Peng,&nbsp;Feng Xu,&nbsp;Zewei Liu","doi":"10.1016/j.cjche.2024.11.013","DOIUrl":"10.1016/j.cjche.2024.11.013","url":null,"abstract":"<div><div>Adsorptive separation holds important prospect for the challenging recovery of C₂H₆ and C₃H₈ from natural gas and the separation efficiency is primarily determined by a high-performance adsorbent. In this work, we reported the synthesis of a novel porous organic polymer, FOSU-POP-1 for the separation of CH₄/C₂H₆/C₃H₈. The FOSU-POP-1 was synthesized from tetrakis(4-azidophenyl)methane and 1,3,5-triethynylbenzene <em>via</em> click reaction with a Brunauer–Emmett–Teller (BET) surface area of 1038 m²·g⁻¹. Exhibiting stronger affinity towards C₃H₈ and C₂H₆ than CH₄, 2.85 mmol·g⁻¹ for C₃H₈ and 2.14 mmol·g⁻¹ for C₂H₆ were achieved on the FOSU-POP-1 at 0.1 MPa, 298 K, with an ideal adsorbed solution theory selectivity of 227 for C₃H₈/CH₄. The breakthrough experiment confirmed the good dynamic separation performance and recyclability of FOSU-POP-1 for CH₄/C₂H₆/C₃H₈ ternary mixture. The density functional theory calculation further revealed that the N atom in triazole ring interacted strongly with the C₃H₈ and C₂H₆. This work highlighted the promising capability of FOSU-POP-1 for efficiently separating CH₄/C₂H₆/C₃H₈ mixture.</div></div>","PeriodicalId":9966,"journal":{"name":"Chinese Journal of Chemical Engineering","volume":"79 ","pages":"Pages 252-259"},"PeriodicalIF":3.7,"publicationDate":"2025-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143580597","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Synergistic effect between nitrogen-doped sites and metal chloride for carbon supported extra-low mercury catalysts in acetylene hydrochlorination","authors":"Yiyang Qiu ,&nbsp;Chong Liu ,&nbsp;Xueting Meng ,&nbsp;Yuesen Liu ,&nbsp;Jiangtao Fan ,&nbsp;Guojun Lan ,&nbsp;Ying Li","doi":"10.1016/j.cjche.2024.11.007","DOIUrl":"10.1016/j.cjche.2024.11.007","url":null,"abstract":"<div><div>Carbon-supported mercury catalysts are extensively employed in calcium carbide-based polyvinyl chloride (PVC) industries, but the usage of mercury-based catalysts can pose an environmental threat due to the release of mercury into the surrounding area during the operation period. In this study, a highly active and stable mercury-based catalyst was developed, utilizing the nitrogen atom of the support as the anchor site to enhance the interaction between active sites (HgCl₂) and the carbon support (N-AC). Thermal loss rate testing and thermogravimetric analysis results demonstrate that, compared to commercial activated carbon, N-doped carbon can effectively increase the heat stability of HgCl₂. The obtained mercury-based catalysts (HgCl₂/N-AC) exhibit significant catalytic performance, achieving 2.5 times the C₂H₂ conversion of conventional HgCl₂/AC catalysts. Experimental analysis combined with theoretical calculations reveals that, contrary to the Eley-Rideal (ER) mechanism of HgCl₂/AC, the HgCl₂/N-AC catalyst follows the Langmuir-Hinshelwood (LH) adsorption mechanism. The nitrogen sites and HgCl₂ on the catalyst enhance the adsorption capabilities of the HCl and C₂H₂, thereby improving the catalytic performance. Based on the modification of the active center by these solid ligands, the loading amount of HgCl₂ on the catalyst can be further reduced from the current 6.5% to 3%. Considering the absence of successful industrial applications for mercury-free catalysts, and based on the current annual consumption of commercial mercury chloride catalysts in the PVC industry, the widespread adoption of this technology could annually reduce the usage of chlorine mercury by 500 tons, making a notable contribution to mercury compliance, reduction, and emissions control in China. It also serves as a bridge between mercury-free and low-mercury catalysts. Moreover, this solid ligand technology can assist in the application research of mercury-free catalysts.</div></div>","PeriodicalId":9966,"journal":{"name":"Chinese Journal of Chemical Engineering","volume":"79 ","pages":"Pages 145-154"},"PeriodicalIF":3.7,"publicationDate":"2025-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143580111","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Zn2+ significantly enhances the performance of petal-like Co-naphthalenetetracarboxylic acid MOF as an anode material for lithium-ion batteries","authors":"Qin Cheng,&nbsp;Pengfei Ma,&nbsp;Ruize Yin,&nbsp;Chaodi Wang,&nbsp;Weiwei Xiong,&nbsp;Zhongyao Duan,&nbsp;Fu Yang,&nbsp;Junhao Zhang","doi":"10.1016/j.cjche.2024.10.034","DOIUrl":"10.1016/j.cjche.2024.10.034","url":null,"abstract":"<div><div>Metal-organic frameworks (MOFs), with their ultrahigh specific surface area, uniformly distributed pores, and tunable structures, are promising candidates for next-generation active electrode materials in lithium-ion batteries (LIBs). However, their application is hindered by poor cycling stability due to structural collapse during charge-discharge cycles. To address this issue, we developed an alloy and multi-solvent thermal method strategy to synthesize Co/Zn bimetallic MOFs based on Naphthalenetetracarboxylic acid (NTCA). The resulting petal-like Co/Zn-NTCA MOF demonstrates outstanding electrochemical performance. The incorporation of zinc ions not only significantly enhances cycling stability but also markedly increases the specific capacity of the anode material. At a current density of 200 mA·g⁻¹, the Co/Zn (2:1)-NTCA MOF demonstrated an impressive reversible capacity of 956 mA·h·g⁻¹ after 150 cycles. Even after 500 cycles, the specific capacity of the electrode remained high, with a value of 438 mA·h·g⁻¹ at a current density of 1000 A·g⁻¹.</div></div>","PeriodicalId":9966,"journal":{"name":"Chinese Journal of Chemical Engineering","volume":"79 ","pages":"Pages 164-171"},"PeriodicalIF":3.7,"publicationDate":"2025-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143580113","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Current advances in distillation processes for fermentative acetone-butanol-ethanol purification","authors":"Xuedan Hou ,&nbsp;Pengfei Zhao ,&nbsp;Xiaohui Lin ,&nbsp;Yunxing Gao ,&nbsp;Huidong Chen ,&nbsp;Di Cai ,&nbsp;Peiyong Qin","doi":"10.1016/j.cjche.2024.08.014","DOIUrl":"10.1016/j.cjche.2024.08.014","url":null,"abstract":"<div><div>Acetone-butanol-ethanol (ABE) fermentation is a primary strategy for producing bio-based <em>n-</em>butanol from abundant renewable biomass. In the typical ABE production chain, distillation is an essential unit for high purity A-B-E productions, but has long been criticized by the energy-inefficient processes due to the extremely low solvents concentration received in the upstream fermentation system. Over the past decades, efforts have been dedicated to developing eco-efficient ABE distillation processes aimed at reducing both energy costs and capital investments. In this review, a comprehensive overview on ABE distillation systems is provided from physico-chemical properties in feed and thermodynamics to the process constructions and applications. The recent trends in distillation sequence construction that fitting with the rapid developed upstream <em>in situ</em> product recovery (ISPR) systems are emphasized. Furthermore, towards developing a more efficient ABE distillation system, the review takes a broad overview of the intensification strategies for ABE distillation. Along with systematic introduction of the key examples, the future directions for ABE distillation techniques development are also discussed towards a sustainable and low-carbon emission biorefineries.</div></div>","PeriodicalId":9966,"journal":{"name":"Chinese Journal of Chemical Engineering","volume":"79 ","pages":"Pages 91-108"},"PeriodicalIF":3.7,"publicationDate":"2025-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143580108","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}