Laborious first-principles calculations and trial-and-error experimentation often fail to meet the demands of rational and efficient catalyst development. This paper introduces an approach that integrates costly labeled data with process reaction mechanisms for catalyst formulation in the high-value conversion of glycerol. We developed an innovative system framework, POCOM, which simultaneously generates the optimal process superstructure and operating conditions to achieve peak conversion rates and desired product specifications. We synergistically combined reaction mechanisms, machine learning, process optimization, and data generation techniques, encapsulating them into a cutting-edge software system specifically designed for catalyst formulation in glycerol selective oxidation. In this process, we identified a previously unreported Pt-ZnO catalyst formulation. The catalyst, with 1.8 wt% Pt and 0.4 wt% ZnO, demonstrated exceptional performance, achieving a glycerol conversion rate of 88% and a glyceric acid selectivity of 80%. This study offers groundbreaking insights and robust data support for the rational design of glycerol oxidation catalysts.
{"title":"Machine learning knowledge-driven Pt-based catalyst design library development for selective oxidation of polyalcohol","authors":"Xin Zhou, Honghua Qin, Zhibo Zhang, Mengzhen Zhu, Hao Yan, Xiang Feng, Lianying Wu, Chaohe Yang, De Chen","doi":"10.1002/aic.18793","DOIUrl":"https://doi.org/10.1002/aic.18793","url":null,"abstract":"Laborious first-principles calculations and trial-and-error experimentation often fail to meet the demands of rational and efficient catalyst development. This paper introduces an approach that integrates costly labeled data with process reaction mechanisms for catalyst formulation in the high-value conversion of glycerol. We developed an innovative system framework, POCOM, which simultaneously generates the optimal process superstructure and operating conditions to achieve peak conversion rates and desired product specifications. We synergistically combined reaction mechanisms, machine learning, process optimization, and data generation techniques, encapsulating them into a cutting-edge software system specifically designed for catalyst formulation in glycerol selective oxidation. In this process, we identified a previously unreported Pt-ZnO catalyst formulation. The catalyst, with 1.8 wt% Pt and 0.4 wt% ZnO, demonstrated exceptional performance, achieving a glycerol conversion rate of 88% and a glyceric acid selectivity of 80%. This study offers groundbreaking insights and robust data support for the rational design of glycerol oxidation catalysts.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"5 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143477873","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}
Proton exchange membrane fuel cells (PEMFCs) are regarded as a cornerstone of next-generation energy conversion technologies due to zero emission and high energy efficiency. However, the high cost and scarcity of conventional Pt-based electrocatalysts hinder its commercialization. Herein, we successfully developed a platinum and cobalt bimetallic covalent organic polymer (Pt-CoNC) electrocatalyst with low Pt loading (0.96 wt%) for the oxygen reduction reaction (ORR) by integrating Pt sites with carbon materials featuring Co-N4 active centers. This unique structural design not only effectively mitigates the high cost associated with Pt-based catalysts but also notably boosts the activity and stability of non-precious metal catalysts. The results verified that the half-wave potential of Pt-CoNC in the acidic ORR was increased by 105 mV as compared with pure cobalt phthalocyanine-based covalent organic polymer (COP-Co). Furthermore, the as-assembled PEMFC device achieved a peak power density of 1.14 W cm−2 under an H2-O2 atmosphere, which is comparable to commercialized 20% Pt/C catalysts.
{"title":"CoN4 active sites coupled with low-loading Pt as advanced oxygen electrocatalyst for proton exchange membrane fuel cells","authors":"Chunzhu Bao, Bolong Yang, Lingling Zhai, Zhonghua Xiang","doi":"10.1002/aic.18763","DOIUrl":"https://doi.org/10.1002/aic.18763","url":null,"abstract":"Proton exchange membrane fuel cells (PEMFCs) are regarded as a cornerstone of next-generation energy conversion technologies due to zero emission and high energy efficiency. However, the high cost and scarcity of conventional Pt-based electrocatalysts hinder its commercialization. Herein, we successfully developed a platinum and cobalt bimetallic covalent organic polymer (Pt-CoNC) electrocatalyst with low Pt loading (0.96 wt%) for the oxygen reduction reaction (ORR) by integrating Pt sites with carbon materials featuring Co-N<sub>4</sub> active centers. This unique structural design not only effectively mitigates the high cost associated with Pt-based catalysts but also notably boosts the activity and stability of non-precious metal catalysts. The results verified that the half-wave potential of Pt-CoNC in the acidic ORR was increased by 105 mV as compared with pure cobalt phthalocyanine-based covalent organic polymer (COP-Co). Furthermore, the as-assembled PEMFC device achieved a peak power density of 1.14 W cm<sup>−2</sup> under an H<sub>2</sub>-O<sub>2</sub> atmosphere, which is comparable to commercialized 20% Pt/C catalysts.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"8 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143486083","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}
Xin Zhang, Xuelu Ma, Hsiao-Chien Chen, Shu Tao, Da Yang, Yingying Liu, Wenwen Gao, Guangxun Sun, Tingyu Chang, Zhidong Wang, Bin Liu, Yongming Chai, Zhi Liu, Yuan Pan
A novel Rh1Co single-atom alloy (SAA) catalyst, in which Rh species are atomically dispersed on Co nanoparticles that are anchored by N-doped carbon (N-C) matrix for hydroformylation of olefins. The Rh1Co SAA/N-C catalyst exhibits high activity towards the hydroformylation of 1-hexene, achieving both nearly 100% conversion and selectivity as well as good cycle stability. It also shows extremely wide substrate generality for at least 17 different types of olefins. A synergistic catalytic mechanism of the Rh1Co SAA/N-C catalyst was discovered that H2 is dissociated on Co sites and Co-H species are facilitated to be generated, CO is also adsorbed and inserted on Co sites that promote the C-C coupling, while the Rh-Co dual sites are beneficial to the co-adsorption of 1-hexene. Theoretical calculations reveal the Rh1Co SAA/N-C catalyst shows a lower rate-determining energy barrier of CO insertion due to the optimized charge distribution of the precursor of CO insertion at Co sites.
{"title":"Carbon matrix anchored Rh1Co single-atom alloy catalyst for robust hydroformylation with wide substrate generality","authors":"Xin Zhang, Xuelu Ma, Hsiao-Chien Chen, Shu Tao, Da Yang, Yingying Liu, Wenwen Gao, Guangxun Sun, Tingyu Chang, Zhidong Wang, Bin Liu, Yongming Chai, Zhi Liu, Yuan Pan","doi":"10.1002/aic.18798","DOIUrl":"https://doi.org/10.1002/aic.18798","url":null,"abstract":"A novel Rh<sub>1</sub>Co single-atom alloy (SAA) catalyst, in which Rh species are atomically dispersed on Co nanoparticles that are anchored by N-doped carbon (N-C) matrix for hydroformylation of olefins. The Rh<sub>1</sub>Co SAA/N-C catalyst exhibits high activity towards the hydroformylation of 1-hexene, achieving both nearly 100% conversion and selectivity as well as good cycle stability. It also shows extremely wide substrate generality for at least 17 different types of olefins. A synergistic catalytic mechanism of the Rh<sub>1</sub>Co SAA/N-C catalyst was discovered that H<sub>2</sub> is dissociated on Co sites and Co-H species are facilitated to be generated, CO is also adsorbed and inserted on Co sites that promote the C-C coupling, while the Rh-Co dual sites are beneficial to the co-adsorption of 1-hexene. Theoretical calculations reveal the Rh<sub>1</sub>Co SAA/N-C catalyst shows a lower rate-determining energy barrier of CO insertion due to the optimized charge distribution of the precursor of CO insertion at Co sites.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"35 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143477872","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 fouling significantly hinders the efficacy of membrane separation engineering in treating oily wastewater. Here, a combined internal and external modification strategy was presented to fabricate a functionalized zwitterionic polyacrylonitrile (PAN) fiber membrane with enhanced antifouling properties for stable emulsion separation. Internally, a zwitterionic polymer betaine methacrylate sulfonate (SBMA) was incorporated into the PAN fiber network to improve hydration, establishing hydration layer barriers to confer fouling resistance. Externally, fluorocarbon small molecules were grafted to create low-surface-energy microregions, imparting the “fouling-release” properties. Due to its fouling resistance and release properties, the resulting membrane (F-PAN@SBMA M) exhibited excellent underwater oil repellency, ultra-low oil adhesion, achieving high separation fluxes (>2000 L m−2 h−1) and efficiencies (>99.1%) for multiple oil-in-water emulsions. Enhanced antifouling properties and high flux recovery rates promoted stable separation performance and membrane regeneration. This modification strategy offers a promising pathway for developing effective membrane separation materials in industrial wastewater treatment.
{"title":"A functionalized zwitterionic PAN fiber membrane with enhanced antifouling for stable emulsion separation","authors":"Hao Chen, Haonan Wu, Yuting Dai, Dongfan Liu, Dongya Yang, Fengxian Qiu, Tao Zhang","doi":"10.1002/aic.18791","DOIUrl":"https://doi.org/10.1002/aic.18791","url":null,"abstract":"Membrane fouling significantly hinders the efficacy of membrane separation engineering in treating oily wastewater. Here, a combined internal and external modification strategy was presented to fabricate a functionalized zwitterionic polyacrylonitrile (PAN) fiber membrane with enhanced antifouling properties for stable emulsion separation. Internally, a zwitterionic polymer betaine methacrylate sulfonate (SBMA) was incorporated into the PAN fiber network to improve hydration, establishing hydration layer barriers to confer fouling resistance. Externally, fluorocarbon small molecules were grafted to create low-surface-energy microregions, imparting the “fouling-release” properties. Due to its fouling resistance and release properties, the resulting membrane (F-PAN@SBMA M) exhibited excellent underwater oil repellency, ultra-low oil adhesion, achieving high separation fluxes (>2000 L m<sup>−2</sup> h<sup>−1</sup>) and efficiencies (>99.1%) for multiple oil-in-water emulsions. Enhanced antifouling properties and high flux recovery rates promoted stable separation performance and membrane regeneration. This modification strategy offers a promising pathway for developing effective membrane separation materials in industrial wastewater treatment.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"34 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143477874","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}
Vincent Dufour-Décieux, Philipp Rehner, Johannes Schilling, Elias Moubarak, Joachim Gross, André Bardow
Physical adsorption is crucial in many industrial processes, prompting researchers to develop new materials for energy-efficient processes. Porous adsorbents are particularly promising due to their design flexibility, and computational screening has accelerated the search for optimal materials. Recently, classical density functional theory (cDFT) has emerged as a faster screening alternative to state-of-the-art computational methods. However, its predictions have not been extensively validated, especially for materials involving strong Coulombic interactions. This article validates cDFT by calculating adsorption properties for over 500 Metal-Organic Frameworks with three adsorbates <span data-altimg="/cms/asset/2b4ac214-7081-4b58-89b7-95daa2eeb1ba/aic18779-math-0001.png"></span><mjx-container ctxtmenu_counter="24" ctxtmenu_oldtabindex="1" jax="CHTML" role="application" sre-explorer- style="font-size: 103%; position: relative;" tabindex="0"><mjx-math aria-hidden="true" location="graphic/aic18779-math-0001.png"><mjx-semantics><mjx-mrow data-semantic-children="0,3" data-semantic-content="0" data-semantic- data-semantic-role="startpunct" data-semantic-speech="left parenthesis CH Subscript 4 Baseline" data-semantic-type="punctuated"><mjx-mo data-semantic- data-semantic-operator="punctuated" data-semantic-parent="4" data-semantic-role="openfence" data-semantic-type="punctuation" style="margin-left: 0.056em; margin-right: 0.056em;"><mjx-c></mjx-c></mjx-mo><mjx-msub data-semantic-children="1,2" data-semantic- data-semantic-parent="4" data-semantic-role="unknown" data-semantic-type="subscript"><mjx-mrow><mjx-mtext data-semantic-annotation="clearspeak:unit" data-semantic-font="normal" data-semantic- data-semantic-parent="3" data-semantic-role="unknown" data-semantic-type="text"><mjx-c></mjx-c><mjx-c></mjx-c></mjx-mtext></mjx-mrow><mjx-script style="vertical-align: -0.15em;"><mjx-mrow size="s"><mjx-mn data-semantic-annotation="clearspeak:simple" data-semantic-font="normal" data-semantic- data-semantic-parent="3" data-semantic-role="integer" data-semantic-type="number"><mjx-c></mjx-c></mjx-mn></mjx-mrow></mjx-script></mjx-msub></mjx-mrow></mjx-semantics></mjx-math><mjx-assistive-mml display="inline" unselectable="on"><math altimg="urn:x-wiley:00011541:media:aic18779:aic18779-math-0001" display="inline" location="graphic/aic18779-math-0001.png" overflow="scroll" xmlns="http://www.w3.org/1998/Math/MathML"><semantics><mrow data-semantic-="" data-semantic-children="0,3" data-semantic-content="0" data-semantic-role="startpunct" data-semantic-speech="left parenthesis CH Subscript 4 Baseline" data-semantic-type="punctuated"><mo data-semantic-="" data-semantic-operator="punctuated" data-semantic-parent="4" data-semantic-role="openfence" data-semantic-type="punctuation" stretchy="false">(</mo><msub data-semantic-="" data-semantic-children="1,2" data-semantic-parent="4" data-semantic-role="unknown" data-semantic-type="subscript"><mrow><mtext data-semantic-="" data-sem
{"title":"Classical density functional theory as a fast and accurate method for adsorption property prediction of porous materials","authors":"Vincent Dufour-Décieux, Philipp Rehner, Johannes Schilling, Elias Moubarak, Joachim Gross, André Bardow","doi":"10.1002/aic.18779","DOIUrl":"https://doi.org/10.1002/aic.18779","url":null,"abstract":"Physical adsorption is crucial in many industrial processes, prompting researchers to develop new materials for energy-efficient processes. Porous adsorbents are particularly promising due to their design flexibility, and computational screening has accelerated the search for optimal materials. Recently, classical density functional theory (cDFT) has emerged as a faster screening alternative to state-of-the-art computational methods. However, its predictions have not been extensively validated, especially for materials involving strong Coulombic interactions. This article validates cDFT by calculating adsorption properties for over 500 Metal-Organic Frameworks with three adsorbates <span data-altimg=\"/cms/asset/2b4ac214-7081-4b58-89b7-95daa2eeb1ba/aic18779-math-0001.png\"></span><mjx-container ctxtmenu_counter=\"24\" ctxtmenu_oldtabindex=\"1\" jax=\"CHTML\" role=\"application\" sre-explorer- style=\"font-size: 103%; position: relative;\" tabindex=\"0\"><mjx-math aria-hidden=\"true\" location=\"graphic/aic18779-math-0001.png\"><mjx-semantics><mjx-mrow data-semantic-children=\"0,3\" data-semantic-content=\"0\" data-semantic- data-semantic-role=\"startpunct\" data-semantic-speech=\"left parenthesis CH Subscript 4 Baseline\" data-semantic-type=\"punctuated\"><mjx-mo data-semantic- data-semantic-operator=\"punctuated\" data-semantic-parent=\"4\" data-semantic-role=\"openfence\" data-semantic-type=\"punctuation\" style=\"margin-left: 0.056em; margin-right: 0.056em;\"><mjx-c></mjx-c></mjx-mo><mjx-msub data-semantic-children=\"1,2\" data-semantic- data-semantic-parent=\"4\" data-semantic-role=\"unknown\" data-semantic-type=\"subscript\"><mjx-mrow><mjx-mtext data-semantic-annotation=\"clearspeak:unit\" data-semantic-font=\"normal\" data-semantic- data-semantic-parent=\"3\" data-semantic-role=\"unknown\" data-semantic-type=\"text\"><mjx-c></mjx-c><mjx-c></mjx-c></mjx-mtext></mjx-mrow><mjx-script style=\"vertical-align: -0.15em;\"><mjx-mrow size=\"s\"><mjx-mn data-semantic-annotation=\"clearspeak:simple\" data-semantic-font=\"normal\" data-semantic- data-semantic-parent=\"3\" data-semantic-role=\"integer\" data-semantic-type=\"number\"><mjx-c></mjx-c></mjx-mn></mjx-mrow></mjx-script></mjx-msub></mjx-mrow></mjx-semantics></mjx-math><mjx-assistive-mml display=\"inline\" unselectable=\"on\"><math altimg=\"urn:x-wiley:00011541:media:aic18779:aic18779-math-0001\" display=\"inline\" location=\"graphic/aic18779-math-0001.png\" overflow=\"scroll\" xmlns=\"http://www.w3.org/1998/Math/MathML\"><semantics><mrow data-semantic-=\"\" data-semantic-children=\"0,3\" data-semantic-content=\"0\" data-semantic-role=\"startpunct\" data-semantic-speech=\"left parenthesis CH Subscript 4 Baseline\" data-semantic-type=\"punctuated\"><mo data-semantic-=\"\" data-semantic-operator=\"punctuated\" data-semantic-parent=\"4\" data-semantic-role=\"openfence\" data-semantic-type=\"punctuation\" stretchy=\"false\">(</mo><msub data-semantic-=\"\" data-semantic-children=\"1,2\" data-semantic-parent=\"4\" data-semantic-role=\"unknown\" data-semantic-type=\"subscript\"><mrow><mtext data-semantic-=\"\" data-sem","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"62 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143462946","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}
Chuanbao Luan, Qifan Cheng, Ningjing Zhu, Andrew Tong, Yinan Zhang, Usina Martha Moatswi, Shiyu Li, Liang Zeng, Liang-Shih Fan
The syngas chemical looping (SCL) process is an advanced thermochemical approach for hydrogen production with in situ carbon capture. This article proposes a novel Ni–Fe bimetallic oxide in a three-reactor chemical looping system. In the moving bed reducer, a mixture of NiO and Fe3O4 is countercurrently reduced by syngas to Ni and Fe/FeO. In the oxidizer, the Fe/FeO mixture is oxidized back to Fe3O4 by steam, producing high-purity H2, while Ni remains unchanged. In the combustor, Ni is oxidized to NiO by air to supply heat, while Fe3O4 is maintained without further oxidation to Fe2O3. The reducer's operating conditions are optimized using the operating line diagram method and the multistage equilibrium model. Process simulation results show that the Ni–Fe oxygen carrier can increase blue hydrogen production efficiency by more than 5% compared to the Fe-based SCL process, while ensuring a carbon capture rate of over 99%.
{"title":"Syngas chemical looping process: Ni–Fe bimetallic oxygen carriers for maximizing blue hydrogen yield","authors":"Chuanbao Luan, Qifan Cheng, Ningjing Zhu, Andrew Tong, Yinan Zhang, Usina Martha Moatswi, Shiyu Li, Liang Zeng, Liang-Shih Fan","doi":"10.1002/aic.18774","DOIUrl":"https://doi.org/10.1002/aic.18774","url":null,"abstract":"The syngas chemical looping (SCL) process is an advanced thermochemical approach for hydrogen production with <i>in situ</i> carbon capture. This article proposes a novel Ni–Fe bimetallic oxide in a three-reactor chemical looping system. In the moving bed reducer, a mixture of NiO and Fe<sub>3</sub>O<sub>4</sub> is countercurrently reduced by syngas to Ni and Fe/FeO. In the oxidizer, the Fe/FeO mixture is oxidized back to Fe<sub>3</sub>O<sub>4</sub> by steam, producing high-purity H<sub>2</sub>, while Ni remains unchanged. In the combustor, Ni is oxidized to NiO by air to supply heat, while Fe<sub>3</sub>O<sub>4</sub> is maintained without further oxidation to Fe<sub>2</sub>O<sub>3</sub>. The reducer's operating conditions are optimized using the operating line diagram method and the multistage equilibrium model. Process simulation results show that the Ni–Fe oxygen carrier can increase blue hydrogen production efficiency by more than 5% compared to the Fe-based SCL process, while ensuring a carbon capture rate of over 99%.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"21 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-02-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143462374","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}
Molybdenum (Mo) serves as the key site in the nitrogenase enzyme, catalyzing the conversion of N2 into NH3 under ambient conditions. However, the strong affinity of Mo sites for N2 hinders H2 adsorption due to the competitive nature of N2 and H2 on a single site, resulting in an unsatisfactory ammonia synthesis performance. Here, we propose an approach of intervening C60 layer as a second site for H2 adsorption on two-dimensional Mo2CTx. The C60 layer thickness is readily tunable by varying its loading content. An optimal C60 layer significantly enhances the electronic interaction between the C60 layer and the Mo2CTx layer, leading to a remarkable decrease in the work function and an increase in the electron density of Mo atoms. Therefore, the separate adsorption of N2 and H2 on distinct sites is substantially facilitated. The present work offers insights into the correlation between structure and performance in NH3 synthesis catalysts.
{"title":"Enhanced layer-layer interaction via a tunable C60 layer in Mo2CTx-based catalyst for ammonia synthesis","authors":"Yangyu Zhang, Yanliang Zhou, Xuanbei Peng, Ming Chen, Jiaxin Li, Mingyuan Zhang, Tianhua Zhang, Jun Ni, Lirong Zheng, Xiuyun Wang, Lilong Jiang","doi":"10.1002/aic.18789","DOIUrl":"https://doi.org/10.1002/aic.18789","url":null,"abstract":"Molybdenum (Mo) serves as the key site in the nitrogenase enzyme, catalyzing the conversion of N<sub>2</sub> into NH<sub>3</sub> under ambient conditions. However, the strong affinity of Mo sites for N<sub>2</sub> hinders H<sub>2</sub> adsorption due to the competitive nature of N<sub>2</sub> and H<sub>2</sub> on a single site, resulting in an unsatisfactory ammonia synthesis performance. Here, we propose an approach of intervening C<sub>60</sub> layer as a second site for H<sub>2</sub> adsorption on two-dimensional Mo<sub>2</sub>CT<sub><i>x</i></sub>. The C<sub>60</sub> layer thickness is readily tunable by varying its loading content. An optimal C<sub>60</sub> layer significantly enhances the electronic interaction between the C<sub>60</sub> layer and the Mo<sub>2</sub>CT<sub><i>x</i></sub> layer, leading to a remarkable decrease in the work function and an increase in the electron density of Mo atoms. Therefore, the separate adsorption of N<sub>2</sub> and H<sub>2</sub> on distinct sites is substantially facilitated. The present work offers insights into the correlation between structure and performance in NH<sub>3</sub> synthesis catalysts.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"66 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-02-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143462445","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}
Energy-efficient pressure swing adsorption (PSA), a technology boosted by extensive research on emerging adsorbents, is a potential alternative to ethylene purification. We investigated, for the first time, the scale-up synthesis, shaping, and high-pressure ethylene-adsorption performance of an ultra-microporous adsorbent, CPL-1-NH2, with an S-type isotherm for ethylene. Based on the static adsorption data and kilogram-scale breakthrough experiments on the shaped CPL-1-NH2, vacuum PSA (VPSA) simulation processes were designed to purify ethylene from a C2H4/C2H6 mixture. Critical variables were investigated and analyzed systematically to increase the purity and recovery of the ethylene product. After parameter optimization, high ethylene purity (99.91%), excellent ethylene recovery (74%), and productivity (1.8 mol kg−1 h−1) were achieved in the 80/20 (C2H4/C2H6, v/v) VPSA simulation. This study reveals that porous materials with flexible isotherms and rapid regeneration ability are desirable for PSA from an engineering perspective.
{"title":"Polymer-grade ethylene production via VPSA simulation with a scalable and shaped ultra-microporous adsorbent","authors":"Yechen Liu, Cong Yu, Kun Lu, Tangyin Wu, Rimin You, Xian Suo, Lifeng Yang, Xili Cui, Huabin Xing","doi":"10.1002/aic.18759","DOIUrl":"https://doi.org/10.1002/aic.18759","url":null,"abstract":"Energy-efficient pressure swing adsorption (PSA), a technology boosted by extensive research on emerging adsorbents, is a potential alternative to ethylene purification. We investigated, for the first time, the scale-up synthesis, shaping, and high-pressure ethylene-adsorption performance of an ultra-microporous adsorbent, CPL-1-NH<sub>2</sub>, with an S-type isotherm for ethylene. Based on the static adsorption data and kilogram-scale breakthrough experiments on the shaped CPL-1-NH<sub>2</sub>, vacuum PSA (VPSA) simulation processes were designed to purify ethylene from a C<sub>2</sub>H<sub>4</sub>/C<sub>2</sub>H<sub>6</sub> mixture. Critical variables were investigated and analyzed systematically to increase the purity and recovery of the ethylene product. After parameter optimization, high ethylene purity (99.91%), excellent ethylene recovery (74%), and productivity (1.8 mol kg<sup>−1</sup> h<sup>−1</sup>) were achieved in the 80/20 (C<sub>2</sub>H<sub>4</sub>/C<sub>2</sub>H<sub>6</sub>, v/v) VPSA simulation. This study reveals that porous materials with flexible isotherms and rapid regeneration ability are desirable for PSA from an engineering perspective.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"15 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-02-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143462944","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}
Operational uncertainties and disruptions present significant challenges in maintaining the resilience and sustainability of pharmaceutical supply chains. Ensuring efficient operations, minimizing emissions, and enhancing distribution reliability are essential for sustainable supply chain performance. This work examines the challenges posed by uncertainty and disruption in the pharmaceutical supply chain, utilizing stochastic optimization and downside risk to formulate mitigation strategies. Specifically, the study compares the solutions of risk-neutral and risk-averse objectives across three key areas: cost, environmental impact, and service level. Solutions from each approach highlight trade-offs: the risk-neutral solution offers better objective values, while the risk-averse one ensures robustness across scenarios but at a higher cost. The multiobjective analysis demonstrates that considering risk is advantageous, as the benefits of robustness outweigh the associated costs. Overall, the results highlight that risk-averse optimization offers strategic advantages for developing robust and sustainable pharmaceutical supply chains in the face of uncertainty and disruption.
{"title":"Optimization of pharmaceutical supply chains: Navigating disruptions and operational uncertainty utilizing risk measures","authors":"Oluwadare Badejo, Marianthi Ierapetritou","doi":"10.1002/aic.18770","DOIUrl":"https://doi.org/10.1002/aic.18770","url":null,"abstract":"Operational uncertainties and disruptions present significant challenges in maintaining the resilience and sustainability of pharmaceutical supply chains. Ensuring efficient operations, minimizing emissions, and enhancing distribution reliability are essential for sustainable supply chain performance. This work examines the challenges posed by uncertainty and disruption in the pharmaceutical supply chain, utilizing stochastic optimization and downside risk to formulate mitigation strategies. Specifically, the study compares the solutions of risk-neutral and risk-averse objectives across three key areas: cost, environmental impact, and service level. Solutions from each approach highlight trade-offs: the risk-neutral solution offers better objective values, while the risk-averse one ensures robustness across scenarios but at a higher cost. The multiobjective analysis demonstrates that considering risk is advantageous, as the benefits of robustness outweigh the associated costs. Overall, the results highlight that risk-averse optimization offers strategic advantages for developing robust and sustainable pharmaceutical supply chains in the face of uncertainty and disruption.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"13 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-02-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143435677","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 this article, a generalized optimization framework is proposed for the synthesis of thermally coupled distillation systems within an equation-oriented environment. The proposed framework consists of three components: an efficient superstructure representation, a novel mathematical formulation, and the associated solution algorithm, encompassing a broad range of alternatives. The mathematical model is developed using conditional statements to activate specific sets of equations, effectively addressing existing zero-flow issues. The synthesis problem is formulated as a Mixed Integer Nonlinear Programming problem, which is optimized using our previously developed Feasible Path-Based Branch and Bound method, coupled with an improved Sequential Quadratic Programming algorithm. The computational studies demonstrate that the proposed optimization framework successfully solves complex benchmark problems for separating zeotropic multicomponent mixtures within reasonable computational time with good convergence performance from easily selected starting points. The optimal configuration generated leads to a reduction in total annualized cost ranging from 3.5% to 45%.
{"title":"Generalized optimization framework for synthesis of thermally coupled distillation columns","authors":"Chao Liu, Yingjie Ma, Jie Li","doi":"10.1002/aic.18776","DOIUrl":"https://doi.org/10.1002/aic.18776","url":null,"abstract":"In this article, a generalized optimization framework is proposed for the synthesis of thermally coupled distillation systems within an equation-oriented environment. The proposed framework consists of three components: an efficient superstructure representation, a novel mathematical formulation, and the associated solution algorithm, encompassing a broad range of alternatives. The mathematical model is developed using conditional statements to activate specific sets of equations, effectively addressing existing zero-flow issues. The synthesis problem is formulated as a Mixed Integer Nonlinear Programming problem, which is optimized using our previously developed Feasible Path-Based Branch and Bound method, coupled with an improved Sequential Quadratic Programming algorithm. The computational studies demonstrate that the proposed optimization framework successfully solves complex benchmark problems for separating zeotropic multicomponent mixtures within reasonable computational time with good convergence performance from easily selected starting points. The optimal configuration generated leads to a reduction in total annualized cost ranging from 3.5% to 45%.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"80 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-02-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143435679","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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