Methods for accurate and efficient protein quantification are crucial in the fields of biomanufacturing, synthetic biology and protein development for optimizing related bioprocesses. Herein, we developed a fluorescent probe, FL-NO2, composed of fluorescein linked to dinitroethylene groups, enabling site-specific covalent labeling of cysteine residues. This probe exhibits high specificity for CPGC-tagged proteins, and the impacts of the location of the inserted dual-Cysteine tag, as well as the introduction of a flexible GGGGS linker, on the protein activity and the labeling efficiency were investigated to extend the practical applicability of this fluorescent tool. Using FL-NO2 as a fluorescence-guided expression platform for in situ protein detection during bacterial fermentation allowed the key parameter optimization. Moreover, this fluorescence-guided platform enabled high-throughput screening of promoter libraries overcoming the labor-intensive limitations of traditional protein expression analysis. This work provides a platform that facilitates the development of in situ protein quantification and high-throughput protein engineering techniques.
{"title":"Dual-cysteine tag-directed fluorescence platform for high-throughput screening of E. coli protein expression systems","authors":"Yiming Ma, Zhuangzhuang Huang, Yuanbo Wang, Sheng Lu, Fang Wang, Bin Wu, Xiaoqiang Chen","doi":"10.1002/aic.70248","DOIUrl":"https://doi.org/10.1002/aic.70248","url":null,"abstract":"Methods for accurate and efficient protein quantification are crucial in the fields of biomanufacturing, synthetic biology and protein development for optimizing related bioprocesses. Herein, we developed a fluorescent probe, <b>FL-NO</b><sub><b>2</b></sub>, composed of fluorescein linked to dinitroethylene groups, enabling site-specific covalent labeling of cysteine residues. This probe exhibits high specificity for CPGC-tagged proteins, and the impacts of the location of the inserted dual-Cysteine tag, as well as the introduction of a flexible GGGGS linker, on the protein activity and the labeling efficiency were investigated to extend the practical applicability of this fluorescent tool. Using <b>FL-NO</b><sub><b>2</b></sub> as a fluorescence-guided expression platform for in situ protein detection during bacterial fermentation allowed the key parameter optimization. Moreover, this fluorescence-guided platform enabled high-throughput screening of promoter libraries overcoming the labor-intensive limitations of traditional protein expression analysis. This work provides a platform that facilitates the development of in situ protein quantification and high-throughput protein engineering techniques.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"7 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2026-01-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146044752","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}
Membrane reactors (MRs) are widely recognized for enhancing thermodynamically limited reactions by continuously removing a product. However, how such in situ selective separation directly impacts intrinsic reaction kinetics and mechanisms has remained ambiguous and lacks direct spectroscopic evidence. Here, we address this fundamental question using a MR integrating a commercial Cu/ZnO/Al2O3 catalyst with carbon molecular sieve (CMS) membranes for methanol steam reforming. The CMS membrane-based MR exhibits a remarkable one-fold enhancement in methanol conversion over a conventional reactor at 180°C, while simultaneously reducing CO selectivity by 61.3%. Crucially, in situ Fourier Transform Infrared Spectroscopy provides direct evidence that this enhancement stems from a profound kinetic acceleration of the rate-determining methoxy dehydrogenation step. This acceleration is driven by efficient removal of H2, which alleviates product inhibition on the catalyst's active sites. This work elucidates a powerful kinetic promotion mechanism, shifting the paradigm of membrane catalysis beyond its thermodynamic role.
{"title":"Beyond equilibrium shift: Unveiling the kinetic promotion in a methanol steam reforming membrane reactor","authors":"Haoyuan Gu, Lisha Wang, Linfeng Lei, Minghui Zhu, Zhi Xu","doi":"10.1002/aic.70257","DOIUrl":"https://doi.org/10.1002/aic.70257","url":null,"abstract":"Membrane reactors (MRs) are widely recognized for enhancing thermodynamically limited reactions by continuously removing a product. However, how such in situ selective separation directly impacts intrinsic reaction kinetics and mechanisms has remained ambiguous and lacks direct spectroscopic evidence. Here, we address this fundamental question using a MR integrating a commercial Cu/ZnO/Al<sub>2</sub>O<sub>3</sub> catalyst with carbon molecular sieve (CMS) membranes for methanol steam reforming. The CMS membrane-based MR exhibits a remarkable one-fold enhancement in methanol conversion over a conventional reactor at 180°C, while simultaneously reducing CO selectivity by 61.3%. Crucially, in situ Fourier Transform Infrared Spectroscopy provides direct evidence that this enhancement stems from a profound kinetic acceleration of the rate-determining methoxy dehydrogenation step. This acceleration is driven by efficient removal of H<sub>2</sub>, which alleviates product inhibition on the catalyst's active sites. This work elucidates a powerful kinetic promotion mechanism, shifting the paradigm of membrane catalysis beyond its thermodynamic role.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"44 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2026-01-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146044755","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}
Ningbo Yu, Shaofei Wang, Min Zhou, Min Xiao, Bo Jin, Hongxia Gao, Zhiwu Liang
Amine-based water-lean solvents serve as energy-efficient absorbents for carbon dioxide (CO2) capture but face paradoxical kinetic challenges, where the mixed solvents inconsistently accelerate or decelerate reaction rates across amine classes. By integrating stopped-flow kinetics, molecular dynamics simulations, and electrostatic potential analysis, we elucidate water modulates CO2 absorption in mixed absorbents systems via amine-specific solvent encapsulation effect for the first time. For primary amines (e.g., monoethanolamine, MEA), water preferentially hydrates nucleophilic nitrogen atoms, forming steric barriers that impede CO2 access and suppress kinetics with increasing hydration. Conversely, secondary amines (e.g., methylaminoethanol, MAE) exhibit oxygen-directed hydration, which weakens nitrogen solvation and enhances electrostatic CO2-amine interactions, accelerating kinetics. A zwitterion-based kinetic model quantifies these solvent-induced activation energy shifts, revealing a universal mechanism validated across diverse solvent systems. This work establishes molecular design principles for tailoring water-lean absorbents, bridging the critical gap between solvent engineering and reaction pathways to advance energy-efficient carbon capture technologies.
{"title":"Unveiling solvent encapsulation-driven kinetic inversion in CO2 absorption by water-lean amine solvents","authors":"Ningbo Yu, Shaofei Wang, Min Zhou, Min Xiao, Bo Jin, Hongxia Gao, Zhiwu Liang","doi":"10.1002/aic.70260","DOIUrl":"https://doi.org/10.1002/aic.70260","url":null,"abstract":"Amine-based water-lean solvents serve as energy-efficient absorbents for carbon dioxide (CO<sub>2</sub>) capture but face paradoxical kinetic challenges, where the mixed solvents inconsistently accelerate or decelerate reaction rates across amine classes. By integrating stopped-flow kinetics, molecular dynamics simulations, and electrostatic potential analysis, we elucidate water modulates CO<sub>2</sub> absorption in mixed absorbents systems via amine-specific solvent encapsulation effect for the first time. For primary amines (e.g., monoethanolamine, MEA), water preferentially hydrates nucleophilic nitrogen atoms, forming steric barriers that impede CO<sub>2</sub> access and suppress kinetics with increasing hydration. Conversely, secondary amines (e.g., methylaminoethanol, MAE) exhibit oxygen-directed hydration, which weakens nitrogen solvation and enhances electrostatic CO<sub>2</sub>-amine interactions, accelerating kinetics. A zwitterion-based kinetic model quantifies these solvent-induced activation energy shifts, revealing a universal mechanism validated across diverse solvent systems. This work establishes molecular design principles for tailoring water-lean absorbents, bridging the critical gap between solvent engineering and reaction pathways to advance energy-efficient carbon capture technologies.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"1 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2026-01-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146044757","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}
Lei Hao, Yeonho Song, Cheng Zhang, Yumei Wang, Haoying Ge, Wen Sun, Jingyun Wang, Jun Soo Kim, Xiaojun Peng, Juyoung Yoon, Haidong Li
Antimicrobial resistance has become a major threat to human health, particularly for Gram-negative bacteria such as Acinetobacter baumannii and Klebsiella pneumoniae. Disruption of membrane integrity is regarded as a promising antimicrobial strategy that does not induce distinct drug resistance, while increasing the internalization of drug doses and mitigating efflux mechanisms. In this study, relying on molecular dynamics (MD) simulations to optimize and confirm the membrane-disrupting activity of photodrugs, we fabricated a series of monomeric (TCn) and dimeric (TCnT) photodrugs (n = 4, 8, 12, and 16), with different alkyl chain lengths, enabling their differing bacterial membrane rupture capabilities of inherent. Notably, based on MD simulations and in vitro experiments, TC8T exhibited enhanced antibacterial efficacy against multiple drug-resistant Gram-negative strains upon white light irradiation, including clinically difficult-to-treat strains. More importantly, TC8T demonstrated robust antimicrobial activity and promoted tissue reconstruction in murine models of wound infection and post-tumor-resection mixed infections.
{"title":"A rational strategy to optimize photodrugs by Molecular Dynamics simulations for killing drug-resistant Gram-negative bacteria","authors":"Lei Hao, Yeonho Song, Cheng Zhang, Yumei Wang, Haoying Ge, Wen Sun, Jingyun Wang, Jun Soo Kim, Xiaojun Peng, Juyoung Yoon, Haidong Li","doi":"10.1002/aic.70238","DOIUrl":"https://doi.org/10.1002/aic.70238","url":null,"abstract":"Antimicrobial resistance has become a major threat to human health, particularly for Gram-negative bacteria such as <i>Acinetobacter baumannii</i> and <i>Klebsiella pneumoniae</i>. Disruption of membrane integrity is regarded as a promising antimicrobial strategy that does not induce distinct drug resistance, while increasing the internalization of drug doses and mitigating efflux mechanisms. In this study, relying on molecular dynamics (MD) simulations to optimize and confirm the membrane-disrupting activity of photodrugs, we fabricated a series of monomeric (TC<sub><i>n</i></sub>) and dimeric (TC<sub><i>n</i></sub>T) photodrugs (<i>n</i> = 4, 8, 12, and 16), with different alkyl chain lengths, enabling their differing bacterial membrane rupture capabilities of inherent. Notably, based on MD simulations and <i>in vitro</i> experiments, TC<sub>8</sub>T exhibited enhanced antibacterial efficacy against multiple drug-resistant Gram-negative strains upon white light irradiation, including clinically difficult-to-treat strains. More importantly, TC<sub>8</sub>T demonstrated robust antimicrobial activity and promoted tissue reconstruction in murine models of wound infection and post-tumor-resection mixed infections.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"142 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2026-01-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146034144","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}
The development of efficient non-noble metal catalysts for ammonia decomposition is critical for advancing hydrogen energy technologies. This study presents a breakthrough in catalyst design by constructing an inverse MgO/Co architecture to synergistically enhance both activity and stability. Through systematic comparison with conventional Co/MgO and unsupported Co nanoparticles, the inverse MgO/Co catalyst achieves 98.7% NH3 conversion at 600°C, with a hydrogen production rate 4.6-fold higher than Co/MgO at 550°C, alongside exceptional stability at 600°C (>90% retention after 100 h). Advanced characterizations (XRD, TEM, XPS, and TPD) reveal that MgO encapsulation of Co nanoparticles generates abundant interfacial oxygen vacancies and strong metal-support interactions, which lower the apparent activation energy to 80.2 kJ mol−1 (vs. 172.3 kJ mol−1 for Co/MgO). These interfacial effects optimize NH3 adsorption energy while facilitating H2 desorption, as evidenced by NH3-TPD and isotopic exchange experiments. The inverse structure simultaneously suppresses Co sintering and stabilizes active metallic Co species, addressing the intrinsic trade-off between activity and durability in conventional catalysts. This work establishes interfacial engineering via inverse design as a universal strategy for high-performance non-precious metal catalysts in hydrogen production systems.
{"title":"Enhanced ammonia decomposition for hydrogen production over an inverse MgO/Co catalyst","authors":"Shigang Li, Yongsheng Li, Bin Dai, Yong Guo","doi":"10.1002/aic.70247","DOIUrl":"https://doi.org/10.1002/aic.70247","url":null,"abstract":"The development of efficient non-noble metal catalysts for ammonia decomposition is critical for advancing hydrogen energy technologies. This study presents a breakthrough in catalyst design by constructing an inverse MgO/Co architecture to synergistically enhance both activity and stability. Through systematic comparison with conventional Co/MgO and unsupported Co nanoparticles, the inverse MgO/Co catalyst achieves 98.7% NH<sub>3</sub> conversion at 600°C, with a hydrogen production rate 4.6-fold higher than Co/MgO at 550°C, alongside exceptional stability at 600°C (>90% retention after 100 h). Advanced characterizations (XRD, TEM, XPS, and TPD) reveal that MgO encapsulation of Co nanoparticles generates abundant interfacial oxygen vacancies and strong metal-support interactions, which lower the apparent activation energy to 80.2 kJ mol<sup>−1</sup> (vs. 172.3 kJ mol<sup>−1</sup> for Co/MgO). These interfacial effects optimize NH<sub>3</sub> adsorption energy while facilitating H<sub>2</sub> desorption, as evidenced by NH<sub>3</sub>-TPD and isotopic exchange experiments. The inverse structure simultaneously suppresses Co sintering and stabilizes active metallic Co species, addressing the intrinsic trade-off between activity and durability in conventional catalysts. This work establishes interfacial engineering via inverse design as a universal strategy for high-performance non-precious metal catalysts in hydrogen production systems.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"142 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2026-01-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146034195","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}
Zakawat Ali, Ju Bai, Wajahat Ali, Mehdi Hassan, Linglong Shan, Xiangping Zhang
Ultra-high permeance and ion–ion selective polyamide (PA) membranes hold immense potential for desalination and brine valorization. To address the inherent limitations of conventional PA membranes that balance permeance and selectivity, we developed a novel host–guest strategy by co-embedding host and guest molecules into the membrane, termed Host–Guest Modulated Interfacial Polymerization (HGMIP). This approach successfully incorporates host–guest molecules into the PA matrix, where host cavities act as artificial water channels, hence enhancing permeance. Simultaneously, the host–guest self-assembly also fine-tunes reaction kinetics and pore size, producing membranes with low molecular weight cut-off (MWCO) and improved surface charge and morphology. Consequently, the optimized PA-H1 ⊃ G and PA-H2 ⊃ G membranes show exceptional size and charge-dependent ion sieving (Li+/Mg2+ = 66, Cl−/SO42− = 289) with improved permeance, highlighting clear advantages over state-of-the-art membranes. This work establishes host–guest chemistry as a versatile platform for engineering PA membranes with tailored nanochannels and surface properties, enabling precise ion–ion separation without compromising permeance.
{"title":"Host–guest assembly engineered nanofiltration membrane for high-efficiency ion–ion separation","authors":"Zakawat Ali, Ju Bai, Wajahat Ali, Mehdi Hassan, Linglong Shan, Xiangping Zhang","doi":"10.1002/aic.70251","DOIUrl":"https://doi.org/10.1002/aic.70251","url":null,"abstract":"Ultra-high permeance and ion–ion selective polyamide (PA) membranes hold immense potential for desalination and brine valorization. To address the inherent limitations of conventional PA membranes that balance permeance and selectivity, we developed a novel host–guest strategy by co-embedding host and guest molecules into the membrane, termed Host–Guest Modulated Interfacial Polymerization (HGMIP). This approach successfully incorporates host–guest molecules into the PA matrix, where host cavities act as artificial water channels, hence enhancing permeance. Simultaneously, the host–guest self-assembly also fine-tunes reaction kinetics and pore size, producing membranes with low molecular weight cut-off (MWCO) and improved surface charge and morphology. Consequently, the optimized PA-H1 ⊃ G and PA-H2 ⊃ G membranes show exceptional size and charge-dependent ion sieving (Li<sup>+</sup>/Mg<sup>2+</sup> = 66, Cl<sup>−</sup>/SO<sub>4</sub><sup>2−</sup> = 289) with improved permeance, highlighting clear advantages over state-of-the-art membranes. This work establishes host–guest chemistry as a versatile platform for engineering PA membranes with tailored nanochannels and surface properties, enabling precise ion–ion separation without compromising permeance.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"30 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2026-01-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146034142","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}
In proton exchange membrane (PEM) water electrolysis, H 2 content in O 2 (HiO) caused by H 2 diffusion from cathode to anode is a critical safety parameter, yet current research exhibits inconsistencies in HiO values and curve patterns. This study employs dual‐scale analysis to investigate HiO evolution mechanisms. From a temporal perspective, we reproduce all HiO curve types observed in the literature by controlling operation time. HiO increases with extended operation duration due to PEM water channel enlargement. Cathode water output emerges as an effective descriptor for water channel sizes and HiO. From a spatial perspective, catalyst layers (CLs) dominate at low current densities by influencing H 2 permeation driving force. PEM water channels contribute at medium current densities via diffusion resistance. At high current densities, CLs—porous transport layers interface become dominant due to local H 2 supersaturation. This work provides the first systematic framework for understanding HiO mechanisms, unifying conflicting literature findings.
{"title":"Breaking the H 2 ‐in‐ O 2 code: Dual‐scale analysis reveals dynamic H 2 permeation mechanisms in PEM water electrolysis","authors":"Zhuolin Yuan, Aidong Tan, Jiwei Shan, Zhang Liu, Chang Liu, Ping Liu, Jianguo Liu","doi":"10.1002/aic.70252","DOIUrl":"https://doi.org/10.1002/aic.70252","url":null,"abstract":"In proton exchange membrane (PEM) water electrolysis, H <jats:sub>2</jats:sub> content in O <jats:sub>2</jats:sub> (HiO) caused by H <jats:sub>2</jats:sub> diffusion from cathode to anode is a critical safety parameter, yet current research exhibits inconsistencies in HiO values and curve patterns. This study employs dual‐scale analysis to investigate HiO evolution mechanisms. From a temporal perspective, we reproduce all HiO curve types observed in the literature by controlling operation time. HiO increases with extended operation duration due to PEM water channel enlargement. Cathode water output emerges as an effective descriptor for water channel sizes and HiO. From a spatial perspective, catalyst layers (CLs) dominate at low current densities by influencing H <jats:sub>2</jats:sub> permeation driving force. PEM water channels contribute at medium current densities via diffusion resistance. At high current densities, CLs—porous transport layers interface become dominant due to local H <jats:sub>2</jats:sub> supersaturation. This work provides the first systematic framework for understanding HiO mechanisms, unifying conflicting literature findings.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"1 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2026-01-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146043171","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}
Mixed‐matrix metal–organic frameworks (MMMOF) membranes combine the advantages of polymeric materials and metal–organic frameworks (MOFs) to enhance molecular separations. However, achieving optimal separation performance depends on the characteristics of the MOFs and their subsequent impact on channel accessibility. Herein, we incorporated geometrically engineered rigid lattices of Cu 2 (pzdc) 2 (pyz) nanosheets with optimized orientation in 6FDA‐DAM to maximize the exposure of molecular‐sieving pores. These engineered Cu 2 (pzdc) 2 (pyz) frameworks formed a rigid triangular structure exhibiting 35% higher CO 2 /CH 4 adsorption selectivity than the pristine MOFs. Furthermore, the oriented MMMOF membranes demonstrated a 104% increase in CO 2 /CH 4 selectivity compared to pure polymer membranes, while maintaining a high CO 2 permeability of 2061 Barrer, surpassing the 2018 mixed‐gas upper bound. This work demonstrates that synergistic control of framework rigidity and oriented pore alignment is a powerful strategy to overcome the “trade‐off” between permeability and selectivity, providing new inspiration for the design of high‐performance molecular sieving membranes.
{"title":"Oriented mixed‐matrix metal–organic framework membranes with geometrically engineered rigid lattice for gas separation","authors":"Qing Li, Kai Qu, Zhiyuan Yi, Linlong Zhou, Shuyun Gu, Zhi Xu","doi":"10.1002/aic.70256","DOIUrl":"https://doi.org/10.1002/aic.70256","url":null,"abstract":"Mixed‐matrix metal–organic frameworks (MMMOF) membranes combine the advantages of polymeric materials and metal–organic frameworks (MOFs) to enhance molecular separations. However, achieving optimal separation performance depends on the characteristics of the MOFs and their subsequent impact on channel accessibility. Herein, we incorporated geometrically engineered rigid lattices of Cu <jats:sub>2</jats:sub> (pzdc) <jats:sub>2</jats:sub> (pyz) nanosheets with optimized orientation in 6FDA‐DAM to maximize the exposure of molecular‐sieving pores. These engineered Cu <jats:sub>2</jats:sub> (pzdc) <jats:sub>2</jats:sub> (pyz) frameworks formed a rigid triangular structure exhibiting 35% higher CO <jats:sub>2</jats:sub> /CH <jats:sub>4</jats:sub> adsorption selectivity than the pristine MOFs. Furthermore, the oriented MMMOF membranes demonstrated a 104% increase in CO <jats:sub>2</jats:sub> /CH <jats:sub>4</jats:sub> selectivity compared to pure polymer membranes, while maintaining a high CO <jats:sub>2</jats:sub> permeability of 2061 Barrer, surpassing the 2018 mixed‐gas upper bound. This work demonstrates that synergistic control of framework rigidity and oriented pore alignment is a powerful strategy to overcome the “trade‐off” between permeability and selectivity, providing new inspiration for the design of high‐performance molecular sieving membranes.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"13 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2026-01-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146043181","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}
Xiaohu Ge, Ping Hu, Yueqiang Cao, Hao Jiang, Jing Zhang, Gang Qian, Xinggui Zhou, De Chen, Xuezhi Duan
Selective hydrogenation of propyne is essential for producing polymer‐grade propylene, yet achieving high selectivity with non‐precious metal catalysts remains challenging. Here, we report a structurally ordered Ni 3 Sn 2 intermetallic catalyst synthesized via topological transformation of NiSn(OH) 6 @Ni/Mg/Al layered double hydroxides. Structural characterization using X‐ray diffraction, high‐resolution transmission electron microscopy, and X‐ray absorption spectroscopy confirms the formation of the hexagonal Ni 3 Sn 2 intermetallic phase, featuring atomically ordered and electronically modulated Ni 1 Sn 2 ensemble sites. The catalyst delivers 98.50% propylene selectivity at near‐complete propyne conversion, markedly outperforming the Ni, Ni 3 Sn, and Ni 3 Sn 4 reference catalysts. Mechanistic insights from temperature‐programmed surface reactions and density functional theory calculations elucidate that the superior performance arises from moderate σ‐type propyne adsorption and kinetically favored propylene desorption on Ni 1 Sn 2 ensemble sites. This work demonstrates a rational intermetallic design strategy for developing high‐performance, non‐noble metal catalysts through precise control of active site geometry and electronic structure.
丙烯的选择性加氢是生产聚合物级丙烯的必要条件，但用非贵金属催化剂实现高选择性仍然具有挑战性。本文报道了通过NiSn(OH) 6 @Ni/Mg/Al层状双氢氧化物的拓扑转化合成的结构有序的Ni 3 Sn 2金属间催化剂。利用X射线衍射、高分辨率透射电子显微镜和X射线吸收光谱进行结构表征，证实了六方Ni 3sn 2金属间相的形成，具有原子有序和电子调制的Ni 1sn 2系综位。在接近完全的丙烯转化中，该催化剂的丙烯选择性为98.50%，明显优于Ni、Ni 3sn和Ni 3sn 4参考催化剂。温度程序化表面反应和密度泛函理论计算的机理分析表明，优异的性能源于适度的σ型丙烯吸附和动力学上有利于丙烯在Ni 1 Sn 2系综上的脱附。这项工作展示了一种合理的金属间设计策略，通过精确控制活性位点的几何形状和电子结构来开发高性能的非贵金属催化剂。
{"title":"Structurally ordered Ni 3 Sn 2 intermetallic catalyst with well‐tuned Ni sites for propyne semihydrogenation","authors":"Xiaohu Ge, Ping Hu, Yueqiang Cao, Hao Jiang, Jing Zhang, Gang Qian, Xinggui Zhou, De Chen, Xuezhi Duan","doi":"10.1002/aic.70245","DOIUrl":"https://doi.org/10.1002/aic.70245","url":null,"abstract":"Selective hydrogenation of propyne is essential for producing polymer‐grade propylene, yet achieving high selectivity with non‐precious metal catalysts remains challenging. Here, we report a structurally ordered Ni <jats:sub>3</jats:sub> Sn <jats:sub>2</jats:sub> intermetallic catalyst synthesized via topological transformation of NiSn(OH) <jats:sub>6</jats:sub> @Ni/Mg/Al layered double hydroxides. Structural characterization using X‐ray diffraction, high‐resolution transmission electron microscopy, and X‐ray absorption spectroscopy confirms the formation of the hexagonal Ni <jats:sub>3</jats:sub> Sn <jats:sub>2</jats:sub> intermetallic phase, featuring atomically ordered and electronically modulated Ni <jats:sub>1</jats:sub> Sn <jats:sub>2</jats:sub> ensemble sites. The catalyst delivers 98.50% propylene selectivity at near‐complete propyne conversion, markedly outperforming the Ni, Ni <jats:sub>3</jats:sub> Sn, and Ni <jats:sub>3</jats:sub> Sn <jats:sub>4</jats:sub> reference catalysts. Mechanistic insights from temperature‐programmed surface reactions and density functional theory calculations elucidate that the superior performance arises from moderate σ‐type propyne adsorption and kinetically favored propylene desorption on Ni <jats:sub>1</jats:sub> Sn <jats:sub>2</jats:sub> ensemble sites. This work demonstrates a rational intermetallic design strategy for developing high‐performance, non‐noble metal catalysts through precise control of active site geometry and electronic structure.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"40 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2026-01-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146043182","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}
Ammonia, as a strategic hydrogen derivative, enables intercontinental energy trade. However, marine applications lack thermal integration studies under spatial and intermittent constraints. Herein, we propose a novel Heat Recovery Multi-Stage Seawater Vacuum Distillation for Electrolytic Water and Ammonia Generation Process (HR-SDEA) that synergistically combines waste heat recovery with multi-stage seawater desalination and ammonia synthesis. This advanced configuration reduces external steam reliance by 40% through repurposing electrolyzer waste heat compared to Seawater vacuum Distillation for Electrolytic water and Ammonia generation process (SDEA), with a modular design suiting offshore environments. Compared with SDEA, the non-renewable energy demand (NED) decreases by 9.56% and greenhouse gas (GHG) emissions reduce by 11.58% per ton of ammonia. Particularly, this configuration reduces carbon emissions by 87.68% and energy consumption by 83.89% over traditional coal-to-ammonia process (CTA) technologies. Combining thermal optimization and modularity, this work breaks bottlenecks for green H2-NH3 chains, enabling viable offshore ammonia.
{"title":"A novel energy integration process for offshore modular green ammonia production systems","authors":"Xin Zhou, Yani Wang, Dongrui Zhang, Mengzhen Zhu, Hao Yan, Yibin Liu, Chaohe Yang, Dehui Deng, Shixiao Fu, Jia Yang, Xuezhi Duan, Xiang Feng, De Chen","doi":"10.1002/aic.70221","DOIUrl":"https://doi.org/10.1002/aic.70221","url":null,"abstract":"Ammonia, as a strategic hydrogen derivative, enables intercontinental energy trade. However, marine applications lack thermal integration studies under spatial and intermittent constraints. Herein, we propose a novel Heat Recovery Multi-Stage Seawater Vacuum Distillation for Electrolytic Water and Ammonia Generation Process (HR-SDEA) that synergistically combines waste heat recovery with multi-stage seawater desalination and ammonia synthesis. This advanced configuration reduces external steam reliance by 40% through repurposing electrolyzer waste heat compared to Seawater vacuum Distillation for Electrolytic water and Ammonia generation process (SDEA), with a modular design suiting offshore environments. Compared with SDEA, the non-renewable energy demand (NED) decreases by 9.56% and greenhouse gas (GHG) emissions reduce by 11.58% per ton of ammonia. Particularly, this configuration reduces carbon emissions by 87.68% and energy consumption by 83.89% over traditional coal-to-ammonia process (CTA) technologies. Combining thermal optimization and modularity, this work breaks bottlenecks for green H<sub>2</sub>-NH<sub>3</sub> chains, enabling viable offshore ammonia.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"16 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2026-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146022180","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}
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