AIChE Journal最新文献_第9页

Kinetics and mechanistic insights into hydrogenative rearrangement of hydroxymethylfurfural over acid-Nickel catalysts 酸-镍催化剂对羟甲基糠醛氢化重排的动力学和机理研究

IF 3.5 3区工程技术

AIChE Journal Pub Date : 2025-04-08 DOI: 10.1002/aic.18855

Fuzeyu Zhong, Weixiao Sun, Xiaohu Ge, Keng Sang, Huihui Qian, Wenyao Chen, Gang Qian, Yueqiang Cao, Jianrong Zeng, Lina Li, Xuezhi Duan, Xinggui Zhou, Jing Zhang

{"title":"Kinetics and mechanistic insights into hydrogenative rearrangement of hydroxymethylfurfural over acid-Nickel catalysts","authors":"Fuzeyu Zhong, Weixiao Sun, Xiaohu Ge, Keng Sang, Huihui Qian, Wenyao Chen, Gang Qian, Yueqiang Cao, Jianrong Zeng, Lina Li, Xuezhi Duan, Xinggui Zhou, Jing Zhang","doi":"10.1002/aic.18855","DOIUrl":"10.1002/aic.18855","url":null,"abstract":"Catalytic hydrogenative rearrangement of furanic aldehydes is crucial for producing biomass-derived cyclopentanone fine chemicals. However, designing highly selective catalysts remains challenging due to the interplay among tandem hydrogenation, ring-opening, aldol condensation, dehydration, and parallel ring-hydrogenation. Here, we employ a single self-assembly step by depositing phosphonic acids (PAs) on conventional Ni catalysts to introduce tunable interfacial Brønsted acid sites (BAS), resulting in an unprecedented 3-hydroxymethyl-cyclopentanone yield of 95.8% from hydroxymethylfurfural. Kinetic studies reveal a one-order-of-magnitude increase in ring-opening rates—the slow step in hydrogenative rearrangement—after PAs modification, accompanied by a drop in the apparent activation energy from 154.1 to 105.4 kJ mol−1. In contrast, the activation energy for the ring-hydrogenation side reaction remains almost unchanged. Theoretical calculations suggest that BAS synergize with adjacent Ni to lower the C–O cleavage barrier by providing protons to attack the hydroxymethyl oxygen atom, which is the key step to initiate ring-opening.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"71 7","pages":""},"PeriodicalIF":3.5,"publicationDate":"2025-04-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143798191","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}

引用次数: 0

Efficient separation of Pd(II) from HCl media by bifunctional thiomorpholinium-based ionic liquids 利用双功能硫代吗啉基离子液体从盐酸介质中高效分离 Pd(II)

IF 3.5 3区工程技术

AIChE Journal Pub Date : 2025-04-08 DOI: 10.1002/aic.18843

Qing Liu, Wanru Wang, Ming Yi, Weichi Chen, Kewen Tang

{"title":"Efficient separation of Pd(II) from HCl media by bifunctional thiomorpholinium-based ionic liquids","authors":"Qing Liu, Wanru Wang, Ming Yi, Weichi Chen, Kewen Tang","doi":"10.1002/aic.18843","DOIUrl":"10.1002/aic.18843","url":null,"abstract":"Bifunctional thiomorpholinium-based ionic liquids were synthesized for the efficient separation of Pd(II) in HCl media. The presence of S atoms in the six-membered ring facilitated the efficient extraction of Pd(II), with a remarkable extraction capacity of 212 mg/g. The extraction mechanism involved anion exchange and coordination. Specifically, PdCl42− preferentially combined with positive N atoms in the thiomorpholinium ring through anion exchange by electrostatic attraction, followed by coordination with the functional sulfur atom to form a stable extracted complex. In addition, the effect of the carbon chain length of the cationic substituent on the extraction performance was systematically investigated to further reveal the structure–activity relationship. More importantly, N,N-dihexyl-thiomorpholinium bis(trifluoromethylsulfonyl)imide exhibited excellent Pd(II) selectivity and reusability, retaining 99.4% extraction efficiency after five extraction-stripping cycles. This study guides the design of ionic liquids-based extractants and offers a solvent-free method for the efficient and environmentally friendly separation of Pd(II).","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"71 7","pages":""},"PeriodicalIF":3.5,"publicationDate":"2025-04-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143798192","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}

引用次数: 0

Constructing grain boundary to stabilize Cu0/Cu+ interfacial sites for efficient CO2 reduction reaction 构建晶界稳定Cu0/Cu+界面位，实现高效CO2还原反应

IF 3.5 3区工程技术

AIChE Journal Pub Date : 2025-04-08 DOI: 10.1002/aic.18829

Saiwu Yang, Yongjun Shen, Xiaoqing Mao, Congcong Li, Zhongliang Liu, Bin Wang, Delin Zhu, Huihui Li, Chunzhong Li

{"title":"Constructing grain boundary to stabilize Cu0/Cu+ interfacial sites for efficient CO2 reduction reaction","authors":"Saiwu Yang, Yongjun Shen, Xiaoqing Mao, Congcong Li, Zhongliang Liu, Bin Wang, Delin Zhu, Huihui Li, Chunzhong Li","doi":"10.1002/aic.18829","DOIUrl":"10.1002/aic.18829","url":null,"abstract":"The electrochemical CO2 reduction reaction (CO2RR) to multi-carbon (C2+) products derived by renewable energy represents a promising strategy for mitigating CO2 emissions. One of the intensively studied strategies is to stabilize Cu+ species on catalysts to facilitate the adsorption of *CO intermediates. However, the reductive environment during CO2RR renders the Cu+ species on the catalyst surface susceptible to reduction to Cu0. Here, we developed a GB-Cu2O-Cu catalyst featuring enriched grain boundaries via an in situ electrochemical reduction process to stabilize Cu+ species, resulting in an abundance of Cu0/Cu+ interfacial active sites. In situ x-ray diffraction (XRD) and Raman spectroscopy further revealed that the presence of grain boundaries effectively shields the Cu+ species on the catalyst surface from undergoing reduction during CO2RR, facilitating the concentration of *CO intermediates and thus promoting C-C dimerization to C2+ products.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"71 7","pages":""},"PeriodicalIF":3.5,"publicationDate":"2025-04-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143797849","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}

引用次数: 0

Flow electrooxidation of chiral alcohols with high enantioselectivity via integrated metal-organic frameworks and aminoxyl radicals 具有高对映选择性的手性醇通过集成金属有机框架和氨基自由基的流动电氧化

IF 3.5 3区工程技术

AIChE Journal Pub Date : 2025-04-04 DOI: 10.1002/aic.18847

Linhan Ren, Jiayuan Li, Suiqin Li, Kai Li, Yuhang Wang, Jieyu Wang, Ying Chen, Jiahui He, Xing Zhong, Jianguo Wang

{"title":"Flow electrooxidation of chiral alcohols with high enantioselectivity via integrated metal-organic frameworks and aminoxyl radicals","authors":"Linhan Ren, Jiayuan Li, Suiqin Li, Kai Li, Yuhang Wang, Jieyu Wang, Ying Chen, Jiahui He, Xing Zhong, Jianguo Wang","doi":"10.1002/aic.18847","DOIUrl":"10.1002/aic.18847","url":null,"abstract":"Chiral compounds play a pivotal role in pharmaceutical chemistry, and the oxidation of chiral alcohols to corresponding carboxylic acids is a crucial step. However, the enantioselectivity is susceptible to degradation due to sensitivity to enol isomerization and racemization. In this study, Ru/S-Ni-MOFs electrocatalysts with high specific surface area were synthesized. After undergoing electrochemical reconfiguration, which combined with 4-acetamido-TEMPO (ACT) as co-catalysts to achieve efficient oxidation of chiral alcohols, with enantioselectivity reaching 99% at industrial-grade current density of 500 mA/cm2. Additionally, 100 g of chiral acid were successfully synthesized with a yield of 98% and an enantioselectivity of 99% in the large-scale electrolyzer. In situ experiments and theoretical calculations demonstrated that S doping shifts the center of d-band toward the Fermi level, which stabilizes ACTH and inhibits the dissociation of OH, thereby enhancing electrocatalytic activity. This study presents an efficient synergistic electrocatalytic strategy for practical large-scale electrosynthesis of chiral carboxylic acid compounds.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"71 7","pages":""},"PeriodicalIF":3.5,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143782428","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}

引用次数: 0

Optimal reactive operation of general topology supply chain and manufacturing networks under disruptions 中断下一般拓扑供应链和制造网络的最优无功运行

IF 3.5 3区工程技术

AIChE Journal Pub Date : 2025-04-03 DOI: 10.1002/aic.18833

Daniel Ovalle, Joshua L. Pulsipher, Yixin Ye, Kyle Harshbarger, Scott Bury, Carl D. Laird, Ignacio E. Grossmann

{"title":"Optimal reactive operation of general topology supply chain and manufacturing networks under disruptions","authors":"Daniel Ovalle, Joshua L. Pulsipher, Yixin Ye, Kyle Harshbarger, Scott Bury, Carl D. Laird, Ignacio E. Grossmann","doi":"10.1002/aic.18833","DOIUrl":"10.1002/aic.18833","url":null,"abstract":"Supply and manufacturing networks in the chemical industry involve diverse processing steps across different locations, rendering their operation vulnerable to disruptions from unplanned events. Optimal responses should consider factors such as product allocation, delayed shipments, and price renegotiation, among other factors. In such context, we propose a multiperiod mixed-integer linear programming model that integrates production, scheduling, shipping, and order management to minimize the financial impact of such disruptions. The model accommodates arbitrary supply chain topologies and incorporates various disruption scenarios, offering adaptability to real-world complexities. A case study from the chemical industry demonstrates the scalability of the model under finer time discretization and explores the influence of disruption types and order management costs on optimal schedules. This approach provides a tractable, adaptable framework for developing responsive operational plans in supply chain and manufacturing networks under uncertainty.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"71 7","pages":""},"PeriodicalIF":3.5,"publicationDate":"2025-04-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/aic.18833","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143782438","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

A differentiable deep learning approach for inverse optimization of hopper flows in particulate manufacturing 颗粒制造中料斗流逆优化的可微深度学习方法

IF 3.5 3区工程技术

AIChE Journal Pub Date : 2025-04-03 DOI: 10.1002/aic.18825

Chengbo Liu, Tingting Liu, Yu Jiang, Yuanye Zhou, Yanjiao Li, Kun Hong, Xizhong Chen

引用次数: 0

Carburization induced phase transition of Ni3In to Ni3InC0.5 intermetallic carbide for acetylene semihydrogenation 渗碳诱导Ni3In向Ni3InC0.5金属间碳化物的相变

IF 3.5 3区工程技术

AIChE Journal Pub Date : 2025-04-02 DOI: 10.1002/aic.18842

Xiaohu Ge, Nina Fei, Yueqiang Cao, Hao Jiang, Jing Zhang, Gang Qian, Xinggui Zhou, Xuezhi Duan

{"title":"Carburization induced phase transition of Ni3In to Ni3InC0.5 intermetallic carbide for acetylene semihydrogenation","authors":"Xiaohu Ge, Nina Fei, Yueqiang Cao, Hao Jiang, Jing Zhang, Gang Qian, Xinggui Zhou, Xuezhi Duan","doi":"10.1002/aic.18842","DOIUrl":"10.1002/aic.18842","url":null,"abstract":"In this work, we develop a carburization strategy to transform hexagonal Ni3In into face-centered cubic Ni3InC0.5 intermetallic carbide, leveraging partially isolated Ni sites for improved acetylene semihydrogenation. The catalyst synthesized via carburization of Ni3In intermetallic compound derived from Ni/In/Mg/Al layered double hydroxides in a C2H2/H2 atmosphere is evidenced to show Ni3InC0.5 intermetallic carbide phase through detailed characterizations, including high-resolution transmission electron microscopy and X-ray absorption spectroscopy. Catalytic tests reveal that the Ni3InC0.5 catalyst achieves 92.0% ethylene selectivity at full acetylene conversion, outperforming the Ni and Ni3In catalysts. Both experimental and theoretical evidence demonstrate that interstitial carbon atoms in Ni3InC0.5 synergize with neighboring In atoms to modify the electronic structure of surface Ni sites via significant hybridization between Ni 3d, In 5p, and C 2p orbitals. These unique features enable higher kinetic favorability of ethylene desorption over its further hydrogenation on the Ni3InC0.5 catalyst and thus contribute to the enhanced semihydrogenation.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"71 7","pages":""},"PeriodicalIF":3.5,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758205","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}

引用次数: 0

Globally optimal basic design of multiple-unit heat exchangers 多机组换热器全局优化基本设计

IF 3.5 3区工程技术

AIChE Journal Pub Date : 2025-04-01 DOI: 10.1002/aic.18838

Miguel J. Bagajewicz, Andre L. M. Nahes, Eduardo M. Queiroz, Diego G. Oliva, Javier A. Francesconi, André L. H. Costa

引用次数: 0

Foaming prediction in pure liquids from dimensionless numbers inspired by the theory of fluid behavior for drops 受液滴流体行为理论启发的无量纲数在纯液体中的泡沫预测

IF 3.5 3区工程技术

AIChE Journal Pub Date : 2025-04-01 DOI: 10.1002/aic.18836

Surya Prakash Tiwari, Robert L. Thompson, Wei Shi, Nicholas Siefert, David Hopkinson, Janice A. Steckel

引用次数: 0

Reactive simulation of an industrial-scale FCC reaction-regeneration full loop system 工业规模催化裂化反应-再生全回路系统的反应模拟