AIChE Journal最新文献_第3页

d-Band center engineering of Cu active sites breaks activity–stability trade-offs in nitrate-to-ammonia electroreduction Cu活性位点的d -波段中心工程打破了硝酸盐-氨电还原中活性-稳定性的权衡

IF 4.4 3区工程技术

AIChE Journal Pub Date : 2026-10-15 Epub Date: 2026-08-12 DOI: 10.1002/aic.70573

Yifei Nie, Yuanjin Li, Hongping Yan, Yaoqi Xie, Qingquan Luo, Qingchun Guo, Shijing Liang, Wei Li, Lilong Jiang

{"title":"d-Band center engineering of Cu active sites breaks activity–stability trade-offs in nitrate-to-ammonia electroreduction","authors":"Yifei Nie, Yuanjin Li, Hongping Yan, Yaoqi Xie, Qingquan Luo, Qingchun Guo, Shijing Liang, Wei Li, Lilong Jiang","doi":"10.1002/aic.70573","DOIUrl":"10.1002/aic.70573","url":null,"abstract":"Copper-based catalysts dominate electrocatalytic nitrate reduction to ammonia (NO3RR), yet suffer from an intrinsic activity-stability trade-off due to strong NH3 intermediates adsorption on Cu active sites, which accelerates catalyst deactivation at high activities. Herein, we regulate the d-band center (εd) of Cu sites through Cu+/Cu0 heterostructure engineering to facilitate NH3 desorption while preserving efficient nitrate conversion. Electrochemical kinetics and DFT calculations identify NH3 desorption as a critical kinetic limitation during NO3RR and reveal that εd downshifting weakens NH3 binding and promotes its removal from the catalyst surface. This electronic modulation simultaneously suppresses Cu leaching (7.9-fold reduction) and lowers the NH3 desorption barrier. The optimized catalyst achieves an NH3 yield rate of 6.6 mg h−1 mgcat−1 with a Faradaic efficiency of 97.9% at −0.8 V in 500 ppm KNO3, while retaining over 95% activity after 24 consecutive cycles. This work establishes electronic-structure regulation as an effective strategy for durable, high-performance NO3RR catalysts.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"72 11","pages":""},"PeriodicalIF":4.4,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148717653","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

Machine learning and physics-informed modeling of cluster coalescence and breakage in gas–solid flows 气固流动中聚结和断裂的机器学习和物理建模

IF 4.4 3区工程技术

AIChE Journal Pub Date : 2026-10-15 Epub Date: 2026-08-17 DOI: 10.1002/aic.70599

Zhikang Zhou, Shanwei Hu, Xinhua Liu

引用次数: 0

Two-dimensional stratified ferrocene-phosphate with adsorption–reduction coupling function for enhanced uranium capture 具有吸附-还原耦合功能的二维层状二茂铁-磷酸增强铀捕获

IF 4.4 3区工程技术

AIChE Journal Pub Date : 2026-10-15 Epub Date: 2026-08-09 DOI: 10.1002/aic.70578

Yue Zhao, Shan Ni, Wang Yao, Yafeng Liu, Wenjie Wang, Huizhou Liu, Liangrong Yang

{"title":"Two-dimensional stratified ferrocene-phosphate with adsorption–reduction coupling function for enhanced uranium capture","authors":"Yue Zhao, Shan Ni, Wang Yao, Yafeng Liu, Wenjie Wang, Huizhou Liu, Liangrong Yang","doi":"10.1002/aic.70578","DOIUrl":"https://doi.org/10.1002/aic.70578","url":null,"abstract":"The development of uranium separation materials is essential to ensure a stable uranium supply for energy and to mitigate environmental risks. We report a two-dimensional ferrocene-vanadyl phosphate composite (fc-VOP) with expanded interlayer spacing (9.8 Å) and adsorption–reduction coupling function, made by solvent-assisted intercalation. This enables efficient uranium capture via optimized interlayer structure and interfacial properties. Interlayer expansion facilitates uranyl ion transport, accelerating adsorption kinetics, while the coupling function elevates interfacial concentration gradients to enhance ion binding, boosting capacity. The fc-VOP shows a theoretical adsorption capacity of 1968.60 mg/g (pH = 4, pure nitrate solution) with equilibrium in 30 min. It also performs well in spiked matrices, achieving 336.4 mg/g in leachate and 248.2 mg/g in seawater. This work provides a viable route to improve 2D phosphate materials for uranyl adsorption and offers mechanistic insights into designing adsorption–reduction coupling materials.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"72 11","pages":""},"PeriodicalIF":4.4,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149177354","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

Shape-based sieving of hexane isomers in liquid-phase by a scalable metal–organic framework 用可伸缩金属有机骨架在液相中对己烷异构体进行基于形状的筛分

IF 4.4 3区工程技术

AIChE Journal Pub Date : 2026-10-15 Epub Date: 2026-08-07 DOI: 10.1002/aic.70591

Yawei Gu, Bingbo Shen, Jingxian Hua, Fuan Guo, Haiqian Lian, Zemin Li, Chen Zhang, Chenkai Gu, Jianbo Hu, Lili Fan, Rujing Hou, Hao Wang, Yichang Pan, Weihong Xing

{"title":"Shape-based sieving of hexane isomers in liquid-phase by a scalable metal–organic framework","authors":"Yawei Gu, Bingbo Shen, Jingxian Hua, Fuan Guo, Haiqian Lian, Zemin Li, Chen Zhang, Chenkai Gu, Jianbo Hu, Lili Fan, Rujing Hou, Hao Wang, Yichang Pan, Weihong Xing","doi":"10.1002/aic.70591","DOIUrl":"10.1002/aic.70591","url":null,"abstract":"The separation of mono- and di-branched alkane isomers is an industrially important yet highly challenging process requiring precise pore structures. Here, we report a scalable metal–organic framework, Ni3(H1.5BTC)2(BTC)(DABCO)3 (denoted as Ni-HDB), featuring an anisotropic, “bat-shaped” pore window that enables precise discrimination of the sterically similar 3-methylpentane (3MP) and 2,3-dimethylbutane (23DMB) pair (~0.3 Å difference in kinetic diameter), thereby enabling efficient separation of mono- and di-branched isomers. Multicomponent vapor- and liquid-phase experiments, supported by molecular simulations, reveal that separation arises from shape-governed molecular accommodation rather than simple size exclusion. Notably, under industrially relevant liquid-phase conditions, a packed column of pelleted Ni-HDB directly produces a high-octane gasoline fraction (RON > 91.5) from a five-component alkane mixture, substantially exceeding the industrial benchmark of 83 for refined hexane mixtures. Combined with scalable synthesis, high stability, and low cost, this work establishes a practical, energy-efficient route for liquid-phase adsorptive upgrading of branched alkanes.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"72 11","pages":""},"PeriodicalIF":4.4,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148687871","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

Covalent organic frameworks for oxygen reduction: Coupling electron, proton, and molecular transport with kinetics 氧还原的共价有机框架：耦合电子、质子和分子传输动力学

IF 4.4 3区工程技术

AIChE Journal Pub Date : 2026-10-15 Epub Date: 2026-08-14 DOI: 10.1002/aic.70574

Min Wang, Yilin Wang, Kunye Zhang, Minghui Wang, Hanlin Cao, Juejin Teng, Yanrong Liu, Hao Wang, Zhongtao Li, Mingbo Wu

{"title":"Covalent organic frameworks for oxygen reduction: Coupling electron, proton, and molecular transport with kinetics","authors":"Min Wang, Yilin Wang, Kunye Zhang, Minghui Wang, Hanlin Cao, Juejin Teng, Yanrong Liu, Hao Wang, Zhongtao Li, Mingbo Wu","doi":"10.1002/aic.70574","DOIUrl":"10.1002/aic.70574","url":null,"abstract":"The oxygen reduction reaction (ORR) remains a central kinetic bottleneck in fuel cells. Its performance depends not only on catalyst activity, but also on electron/proton transfer, oxygen transport, and surface reaction kinetics. Because catalytic reactions and mass transport occur on different timescales, their matching is essential for efficient ORR. Covalent organic frameworks (COFs) have attracted increasing interest in ORR electrocatalysis because of their tunable structures and ordered pores. However, current studies mainly focus on material classification or activity regulation, while the relationship between transport and reaction kinetics remains insufficiently understood. To bridge this gap, this review proposes a transport-reaction coupling framework for COF-based ORR electrocatalysts. By comparing pyrolyzed and non-pyrolyzed COFs, a key principle is revealed: electron, proton, and oxygen transport should be balanced with regulation of the local reaction environment. This review links molecular COF design, multiscale transport, and device performance to guide the design of COF-based ORR electrocatalysts.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"72 11","pages":""},"PeriodicalIF":4.4,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148729057","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

Nitrogen configuration engineering in carbon-encapsulated Ni nanocatalysts for efficient CO2/MgCO3 electroreduction 碳包覆镍纳米催化剂的氮组态工程用于CO2/MgCO3高效电还原

IF 4.4 3区工程技术

AIChE Journal Pub Date : 2026-10-15 Epub Date: 2026-07-26 DOI: 10.1002/aic.70556

Meng Wang, Hongri Suo, Qiuhong Sun, Wenjing Dong, Zhijia Yang, Peisen Li, Jian Zhang, Xiao-Jue Bai, Yufei Zhao

{"title":"Nitrogen configuration engineering in carbon-encapsulated Ni nanocatalysts for efficient CO2/MgCO3 electroreduction","authors":"Meng Wang, Hongri Suo, Qiuhong Sun, Wenjing Dong, Zhijia Yang, Peisen Li, Jian Zhang, Xiao-Jue Bai, Yufei Zhao","doi":"10.1002/aic.70556","DOIUrl":"https://doi.org/10.1002/aic.70556","url":null,"abstract":"Electrocatalytic CO2 reduction into value-added products enables carbon cycling and renewable energy storage. Developing non-precious metal catalysts with high activity, selectivity, and long-term stability remains challenging. Herein, we design nitrogen-doped carbon-encapsulated Ni nanoparticles (Ni-N-C) using layered double hydroxide as precursors. The pyridinic-to-pyrrolic N ratio (Npy/Npr) is tuned by pyrolysis temperature. The optimal Ni-N-C-750 (Npy/Npr ≈1) delivers a CO Faradaic efficiency of 97.8% at −1.5 V versus Ag/AgCl, maintains >80% CO selectivity across a broad current density range, and exhibits >100 h stability. The balanced N configuration optimizes the electronic structure, lowering the *COOH formation barrier while suppressing hydrogen evolution. Furthermore, using MgCO3 as a solid carbon source enables tunable syngas (CO/H2 up to ~0.1) and Mg(OH)2 byproduct, demonstrating the coupling of carbonate conversion with CO2RR. This work establishes nitrogen configuration engineering as a design principle for efficient and durable carbon-encapsulated electrocatalysts, providing a platform for coupling carbonate conversion.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"72 11","pages":""},"PeriodicalIF":4.4,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149177703","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

Lignin barrier reconstruction outweighs delignification in determining enzymatic hydrolysis of pretreated poplar 测定预处理杨树酶解的木质素屏障重建优于去木质素作用

IF 4.4 3区工程技术

AIChE Journal Pub Date : 2026-10-15 Epub Date: 2026-08-06 DOI: 10.1002/aic.70577

Ruoyan Li, Wenna Guan, Ke Zheng, Xiaoxue Zhao, Daihui Zhang, Chenhuan Lai

{"title":"Lignin barrier reconstruction outweighs delignification in determining enzymatic hydrolysis of pretreated poplar","authors":"Ruoyan Li, Wenna Guan, Ke Zheng, Xiaoxue Zhao, Daihui Zhang, Chenhuan Lai","doi":"10.1002/aic.70577","DOIUrl":"10.1002/aic.70577","url":null,"abstract":"Efficient lignin removal is widely considered essential for improving enzymatic hydrolysis of lignocellulose. However, lignin redistribution and structural changes during pretreatment may reconstruct the lignin barrier, impacting enzymatic hydrolysis. In this study, poplar was treated with a sequential hydrothermal–deep eutectic solvent pretreatment (HP–DES) and compared with standalone hydrothermal and DES pretreatments. Despite higher delignification efficiencies, HP-DES-pretreated substrates exhibited substantially lower enzymatic hydrolysis yields (33.5%–55.3%) than single DES-pretreated substrates (41.2%–74.8%). To elucidate this counterintuitive behavior, lignin redistribution, structural evolution, and enzyme–lignin interactions were investigated using microscopic imaging, spectroscopic characterization, and reconstructed lignocellulose experiments. The results revealed that HP-DES pretreatment promoted lignin migration toward the substrate surface, increased the number of phenolic hydroxyl groups, and enhanced lignin condensation, thereby intensifying enzyme non-productive binding. These findings unraveled that lignin barrier reconstruction outweighs delignification in determining enzymatic hydrolysis, giving new insights into effective pretreatment process design.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"72 11","pages":""},"PeriodicalIF":4.4,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148687872","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

Membrane-aided simultaneous reaction–separation for liquid phase products 膜辅助液相产物同时反应分离

IF 4.4 3区工程技术

AIChE Journal Pub Date : 2026-10-15 Epub Date: 2026-08-06 DOI: 10.1002/aic.70589

Yihan Song, Abdulmalik Dahiru, Alan Tirado, Cliff Kowall, Lei Li

{"title":"Membrane-aided simultaneous reaction–separation for liquid phase products","authors":"Yihan Song, Abdulmalik Dahiru, Alan Tirado, Cliff Kowall, Lei Li","doi":"10.1002/aic.70589","DOIUrl":"10.1002/aic.70589","url":null,"abstract":"Conventionally, reaction and separation are conducted as separate steps in liquid-phase manufacturing, with products formed during reaction and subsequently separated from unreacted reagents, solvents, and byproducts. Integrating these steps into a simultaneous reaction–separation process can improve efficiency and reduce costs. Here, we developed a membrane-based reactor that enables reaction and selective product separation simultaneously. We demonstrate the simultaneous reaction–separation of the ionic liquid (IL) [EMIM][NTf2] using a hydrophobic/oleophilic perfluorocarbon-coated membrane, with capillary pressure as the primary separation driving force. Without the post-reaction washing required in conventional decanting, the process achieves comparable IL purity, including lower water content and slightly higher Li+ content, as confirmed by NMR, TGA, and ICP-MS. The separation performance remains stable over multiple reaction–separation cycles. These findings provide a promising strategy for more efficient industrial manufacturing of liquid-phase products.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"72 11","pages":""},"PeriodicalIF":4.4,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/aic.70589","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148687889","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

Sonocatalytic carbon dioxide reduction for syngas production over surface-roughened CuxO catalyst 合成气生产的声催化二氧化碳还原表面粗化的Cu x O催化剂

IF 4.4 3区工程技术

AIChE Journal Pub Date : 2026-10-15 Epub Date: 2026-08-16 DOI: 10.1002/aic.70605

Dong Xia, Yi Qin, Hessan Khalid, Yagya N. Regmi, Laurie A. King, James Kwan

{"title":"Sonocatalytic carbon dioxide reduction for syngas production over surface-roughened CuxO catalyst","authors":"Dong Xia, Yi Qin, Hessan Khalid, Yagya N. Regmi, Laurie A. King, James Kwan","doi":"10.1002/aic.70605","DOIUrl":"10.1002/aic.70605","url":null,"abstract":"The transition to a carbon-circular economy requires efficient technologies for converting CO2 into value-added chemical feedstocks. Sonocatalytic CO2 conversion has recently emerged as a compelling approach to drive this conversion. Here, we report a surface-roughened CuxO catalyst for sonocatalytic CO2 reduction in aqueous media, achieving a marked CO2-to-CO conversion alongside H2 production, yielding tunable syngas (CO/H2) ratios relevant to Fischer–Tropsch and methanol synthesis processes. We demonstrate that the CO/H2 ratio is systematically controlled by varying the solution composition (KHCO3, CH3COOK, and KCl), revealing solution-mediated selectivity as an unexplored lever in CO2 sonocatalytic systems. Prolonged testing in CO2-saturated KHCO3 solutions induced morphological deformations of the CuxO catalyst which were shown to benefit sonolysis, as evidenced by higher CO production rates during long-term operation. Our findings highlight surface-roughened CuxO catalyst for sonocatalytic conversion of CO2-saturated solutions to syngas and introduce solution engineering as a new approach to tune product selectivity.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"72 11","pages":""},"PeriodicalIF":4.4,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/aic.70605","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148729056","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

Promoting the regeneration of polyethylenimine-impregnated sorbents through in situ vapor purge for direct air capture 促进再生聚乙烯亚胺浸渍吸附剂通过原位蒸汽吹扫直接空气捕获

IF 4.4 3区工程技术

AIChE Journal Pub Date : 2026-10-15 Epub Date: 2026-08-08 DOI: 10.1002/aic.70571

Yongqiang Wang, Qiuran Yang, Paul Webley, Guoping Hu, Gang Kevin Li

{"title":"Promoting the regeneration of polyethylenimine-impregnated sorbents through in situ vapor purge for direct air capture","authors":"Yongqiang Wang, Qiuran Yang, Paul Webley, Guoping Hu, Gang Kevin Li","doi":"10.1002/aic.70571","DOIUrl":"10.1002/aic.70571","url":null,"abstract":"Amine-impregnated sorbents (AIS) have been extensively investigated for direct air capture (DAC) due to their high adsorption capacity and selectivity toward atmospheric CO2. However, there has been limited attention given to efficiently recovering the adsorbed CO2 from AIS, leading to the regeneration remaining energy-intensive in DAC systems. Here, we employ a double-layered adsorption configuration, in situ producing vapors using water synergistically harvested from the air to effectively regenerate polyethylenimine-impregnated sorbents. This vapor-promoted regeneration provided a substantial driving force for CO2 desorption at ambient pressure and 105°C, producing water and 99% purity CO2 with a high working capacity of 1.61 mmol/g. Only 8.9 MJ/<math>\u0000 <mrow>\u0000 <msub>\u0000 <mi>kg</mi>\u0000 <mrow>\u0000 <mi>C</mi>\u0000 <msub>\u0000 <mi>O</mi>\u0000 <mn>2</mn>\u0000 </msub>\u0000 </mrow>\u0000 </msub>\u0000 </mrow></math> thermal energy was consumed for sorbent regeneration without the use of vacuum conditions and external purge. This in situ vapor purge enables the recovery of over 95% of the CO2 adsorbed on AIS, paving the way for the practical application of low-cost chemisorbents in DAC.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"72 11","pages":""},"PeriodicalIF":4.4,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148688090","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