AIChE Journal最新文献_第9页

General descriptors for glycerol oxidation to glyceric acid over PtM3‐derived bimetallic catalysts in base‐free medium 在无碱介质中，通过PtM3衍生的双金属催化剂将甘油氧化为甘油酸的一般描述符

IF 3.7 3区工程技术

AIChE Journal Pub Date : 2024-12-16 DOI: 10.1002/aic.18683

Hao Yan, Jiarong Lu, Yaqian Li, Xiang Feng, Xin Zhou, Hui Zhao, Chaohe Yang

{"title":"General descriptors for glycerol oxidation to glyceric acid over PtM3‐derived bimetallic catalysts in base‐free medium","authors":"Hao Yan, Jiarong Lu, Yaqian Li, Xiang Feng, Xin Zhou, Hui Zhao, Chaohe Yang","doi":"10.1002/aic.18683","DOIUrl":"https://doi.org/10.1002/aic.18683","url":null,"abstract":"Exploring efficient Pt‐based catalysts for the selective oxidation of polyol is still a challenge due to the lack of a mechanism‐driven approach. Here, low‐Pt content PdM3 were systematically investigated for glycerol oxidation to glyceric acid (GLYA) by density functional theory (DFT) linear synchronous transit and quadratic synchronous transit (LST/QST) assisted descriptor‐based micro‐kinetic modeling. Results revealed that the PdM3 surface induces the dissociation of O2 and H2O to form a polarized PdM3‐OH* surface, participating in the subsequent adsorption and activation of glycerol and oxygen‐containing intermediates. Moreover, the binding energy of O and H on the PdM3 could be labeled as descriptors describing catalytic selectivity and activity. On this basis, a strong electron reconstruction effect described by EO (−4.5 to −3.0 eV) and appropriate dehydrogenation ability described by EH (−3.5 to −2.5 eV) contribute to the improvement of catalytic performance for the selective oxidation of glycerol to GLYA. This study may give insights into the rational design of high‐efficient Pt‐based catalysts for polyol oxidation.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"3 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2024-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142825183","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

Enhancing H2 production from plasma-assisted methanol steam reforming by catalyst engineering in a MXene membrane reactor 在 MXene 膜反应器中通过催化剂工程提高等离子体辅助甲醇蒸汽转化的 H2 产量

IF 3.5 3区工程技术

AIChE Journal Pub Date : 2024-12-14 DOI: 10.1002/aic.18685

Shaowei Chen, Zong Lu, Jiangqi Niu, Yan Shao, Yi Chen, Yaru Ni, Xiaoying Liu, Xiaoyang Wei, Xiaoxia Ou, Xiaolei Fan, Yanying Wei, Huanhao Chen

引用次数: 0

Synergistic photocatalytic synthesis of H2O2: Mechanistic insights and sustainable applications H2O2 的协同光催化合成：机理认识与可持续应用

IF 3.5 3区工程技术

AIChE Journal Pub Date : 2024-12-14 DOI: 10.1002/aic.18692

Zaixiang Xu, Wenjuan Fang, Fengcang Zhou, Chenghang Jiang, Jingnan Zheng, Yanfeng Li, Shijie Zhang, Zhikang Bao, Qun Cao, Jianguo Wang

{"title":"Synergistic photocatalytic synthesis of H2O2: Mechanistic insights and sustainable applications","authors":"Zaixiang Xu, Wenjuan Fang, Fengcang Zhou, Chenghang Jiang, Jingnan Zheng, Yanfeng Li, Shijie Zhang, Zhikang Bao, Qun Cao, Jianguo Wang","doi":"10.1002/aic.18692","DOIUrl":"10.1002/aic.18692","url":null,"abstract":"The synthesis of hydrogen peroxide (H₂O₂) via photocatalysis represents a sustainable and environmentally friendly approach with significant potential for diverse applications. This study reveals the involvement of a novel triple interplay catalytic cycle in the photocatalytic production of H₂O₂, providing crucial insights into the underlying reaction mechanisms. Utilizing modified carbon nitride (m-CN) as the catalyst, we achieved H₂O₂ concentrations of 3368 mmol L−1 (11.5 wt.%) and a production rate of 4900 mM g cat−1 h−1, demonstrating significant improvements over existing methods. Stability tests and spectroscopic analyses confirmed the robustness of the system over 100 h. Mechanistic studies, including EPR spectroscopy and kinetic analysis, further elucidated the reaction pathways, enhancing our understanding of H₂O₂ synthesis. This research offers a foundation for designing next-generation photocatalytic systems with improved efficiency and selectivity, contributing to the advancement of sustainable H₂O₂ production for cooperative organic synthesis.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"71 3","pages":""},"PeriodicalIF":3.5,"publicationDate":"2024-12-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/aic.18692","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142820955","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

Screening of pure silica zeolites with high ethane/ethylene separation selectivity by simulations and experiments 通过模拟和实验筛选具有高乙烷/乙烯分离选择性的纯硅分子筛

IF 3.5 3区工程技术

AIChE Journal Pub Date : 2024-12-13 DOI: 10.1002/aic.18676

Peixin Zhang, Jianbo Hu, Dengzhuo Zhou, Xiaofei Lu, Lifeng Yang, Liyuan Chen, Xian Suo, Xili Cui, Huabin Xing

{"title":"Screening of pure silica zeolites with high ethane/ethylene separation selectivity by simulations and experiments","authors":"Peixin Zhang, Jianbo Hu, Dengzhuo Zhou, Xiaofei Lu, Lifeng Yang, Liyuan Chen, Xian Suo, Xili Cui, Huabin Xing","doi":"10.1002/aic.18676","DOIUrl":"10.1002/aic.18676","url":null,"abstract":"The advancement of ethane (C2H6)-selective materials offers the potential for developing energy-efficient adsorptive separation processes to obtain high-purity ethylene (C2H4) directly. However, these materials still suffer challenges of low selectivity, high cost, and poor stability. Herein, we presented a commercially scalable and stable MFI topology zeolite material (TS-1) with excellent ideal adsorption solution theory (IAST) selectivity (2.07) and separation potential (0.64 mmol g−1). Polymer-grade ethylene (99.9%) could be afforded with the productivity of 11.5 L kg−1 through the adsorption column packed with TS-1 material. Additionally, pure silica zeolite with DOH topology with excellent IAST selectivity (2.93) and separation potential (1.64 mmol g−1) was discovered by high-throughput screening via the combination of experiments and simulations. These findings highlight that pure silica zeolites hold promise as C2H6-selective adsorbents for large-scale implementation for one-step C2H4 purification.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"71 3","pages":""},"PeriodicalIF":3.5,"publicationDate":"2024-12-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142816389","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

Stabilizing *OH intermediate by fabricating Ni3N-MoN for scalable 5-hydroxymethylfurfural electrooxidation 通过制备Ni3N-MoN来稳定*OH中间体，用于可扩展的5-羟甲基糠醛电氧化

IF 3.5 3区工程技术

AIChE Journal Pub Date : 2024-12-13 DOI: 10.1002/aic.18690

Shaowei Yang, Ying Guo, Jie Yang, Runze Gao, Zhibei Liao, Haidong Shen, Haoxi Wang, Lifeng Jiang, Buxing Han, Qiuyu Zhang, Hepeng Zhang

{"title":"Stabilizing *OH intermediate by fabricating Ni3N-MoN for scalable 5-hydroxymethylfurfural electrooxidation","authors":"Shaowei Yang, Ying Guo, Jie Yang, Runze Gao, Zhibei Liao, Haidong Shen, Haoxi Wang, Lifeng Jiang, Buxing Han, Qiuyu Zhang, Hepeng Zhang","doi":"10.1002/aic.18690","DOIUrl":"10.1002/aic.18690","url":null,"abstract":"Achieving large-scale coupling of organic electrooxidation and the hydrogen evolution reaction, while understanding the competition between organic electrooxidation and oxygen evolution reaction (OER), is a significant challenge. In this study, using Ni3N-MoN/NF, an efficient heterojunction electrocatalyst as both anode and cathode in a 50 cm2 continuous flow reactor, we achieved a total current of ~20 A at 2.6 V. This resulted in the highest single-pass 5-hydroxymethylfurfural conversion efficiency (0.049 mmol cm−2 min−1) and gram-level production of 2,5-furandicarboxylic acid. Theoretical studies revealed that MoN accelerated *OH formation and increased its deprotonation energy barrier, leading to *OH accumulation, effectively promoting organic electrooxidation and inhibiting OER. We anticipate that our foundation in understanding the reaction mechanism and catalyst design strategy can be extended to a wider range of anodic oxidation reactions.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"71 3","pages":""},"PeriodicalIF":3.5,"publicationDate":"2024-12-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142816390","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

Advanced downstream processing for sustainable ethyl acetate production by fermentation 可持续发酵生产乙酸乙酯的先进下游加工

IF 3.5 3区工程技术

AIChE Journal Pub Date : 2024-12-13 DOI: 10.1002/aic.18684

Tamara Janković, Adrie J. J. Straathof, Anton A. Kiss

{"title":"Advanced downstream processing for sustainable ethyl acetate production by fermentation","authors":"Tamara Janković, Adrie J. J. Straathof, Anton A. Kiss","doi":"10.1002/aic.18684","DOIUrl":"10.1002/aic.18684","url":null,"abstract":"Ethyl acetate is a platform chemical conventionally obtained through fossil fuel routes, but more recently its production by fermentation from carbohydrates has been scaled up to a pilot scale. Yet, the complexity of downstream processing (low product concentrations in liquid broth and in off-gas, azeotrope formation, and the presence of microorganisms) may complicate industrial application. This original theoretical study is the first to develop advanced downstream processing, based on process intensification principles, for large-scale recovery (~10 kton/year) of ethyl acetate after fermentation. To minimize product losses, ethyl acetate is separated from both the liquid broth and off-gas. The final purification is performed in a highly integrated azeotropic dividing-wall column. The economic and sustainability analysis shows that using refrigeration for initial product separation from the gas phase is more cost-effective (~0.61 $/kg) and less energy-intensive (2.20–2.40 kWthh/kg) than compression combined with high-pressure condensation using chilled water (1.09 $/kg and 9.98 kWthh/kg).","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"71 3","pages":""},"PeriodicalIF":3.5,"publicationDate":"2024-12-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/aic.18684","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142816391","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

Deep DeePC: Data-enabled predictive control with low or no online optimization using deep learning Deep DeePC：数据支持的预测控制，使用深度学习进行低在线优化或没有在线优化

IF 3.5 3区工程技术

AIChE Journal Pub Date : 2024-12-11 DOI: 10.1002/aic.18644

Xuewen Zhang, Kaixiang Zhang, Zhaojian Li, Xunyuan Yin

{"title":"Deep DeePC: Data-enabled predictive control with low or no online optimization using deep learning","authors":"Xuewen Zhang, Kaixiang Zhang, Zhaojian Li, Xunyuan Yin","doi":"10.1002/aic.18644","DOIUrl":"10.1002/aic.18644","url":null,"abstract":"Data-enabled predictive control (DeePC) is a data-driven control algorithm that utilizes data matrices to form a non-parametric representation of the underlying system, predicting future behaviors and generating optimal control actions. DeePC typically requires solving an online optimization problem, the complexity of which is heavily influenced by the amount of data used, potentially leading to expensive online computation. In this article, we leverage deep learning to propose a highly computationally efficient DeePC approach for general nonlinear processes, referred to as Deep DeePC. Specifically, a deep neural network is employed to learn the DeePC vector operator, which is an essential component of the non-parametric representation of DeePC. This neural network is trained offline using historical open-loop input and output data of the nonlinear process. With the trained neural network, the Deep DeePC framework is formed for online control implementation. At each sampling instant, this neural network directly outputs the DeePC operator, eliminating the need for online optimization as conventional DeePC. The optimal control action is obtained based on the DeePC operator updated by the trained neural network. To address constrained scenarios, a constraint handling scheme is further proposed and integrated with the Deep DeePC to handle hard constraints during online implementation. The efficacy and superiority of the proposed Deep DeePC approach are demonstrated using two benchmark process examples.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"71 3","pages":""},"PeriodicalIF":3.5,"publicationDate":"2024-12-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142804924","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

Designing and screening single-atom alloy catalysts for CO2 reduction to CH3OH via DFT and machine learning 基于DFT和机器学习的单原子合金催化剂的设计与筛选

IF 3.5 3区工程技术

AIChE Journal Pub Date : 2024-12-10 DOI: 10.1002/aic.18678

Wenyu Zhou, Haisong Feng, Shihong Zhou, Mengxin Wang, Yuping Chen, Chenyang Lu, Hao Yuan, Jing Yang, Qun Li, Luxi Tan, Lichun Dong, Yong-Wei Zhang

{"title":"Designing and screening single-atom alloy catalysts for CO2 reduction to CH3OH via DFT and machine learning","authors":"Wenyu Zhou, Haisong Feng, Shihong Zhou, Mengxin Wang, Yuping Chen, Chenyang Lu, Hao Yuan, Jing Yang, Qun Li, Luxi Tan, Lichun Dong, Yong-Wei Zhang","doi":"10.1002/aic.18678","DOIUrl":"10.1002/aic.18678","url":null,"abstract":"Carbon dioxide (CO2) utilization technology is of great significance for achieving carbon neutrality, in which the catalytic materials play crucial roles, and among them, single-atom alloys (SAAs) are of particular interests. In this study, density functional theory (DFT) calculations and machine learning are employed to assess the effectiveness of Cu-, Ag-, and Ni-host SAAs as catalysts for electrochemical CO2 reduction to CH3OH. The Gibbs free energies of 477 elementary reactions across 35 SAAs involved in CO2 reduction are calculated, and by utilizing this dataset, a trained gradient boosting regression model is established with an excellent accuracy. Subsequently, the properties of 46 unknown SAAs are predicted, including their pathways, products, potential-determining steps (PDS), and corresponding Gibbs free energies of the PDS (GPDS). Three promising candidates, ZnCu, AuAg and MoNi, stand out due to their lowest GPDS among Cu-, Ag- and Ni- hosted SAAs, respectively.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"71 3","pages":""},"PeriodicalIF":3.5,"publicationDate":"2024-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142797388","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

Oxime ether photobromination in a photomicroreactor: Process parameters and kinetic modeling 光微反应器中的肟醚光溴化：工艺参数和动力学模型

IF 3.5 3区工程技术

AIChE Journal Pub Date : 2024-12-10 DOI: 10.1002/aic.18693

You Ma, Guozhi Qian, Mohsin Pasha, Yuhan Wang, Jiayi Li, Yuzhe Liu, Saier Liu, Xiao Xue, Min Qiu, Zihao Zhong, Minjing Shang, Jie Zheng, Zhigang Lin, Yuanhai Su

{"title":"Oxime ether photobromination in a photomicroreactor: Process parameters and kinetic modeling","authors":"You Ma, Guozhi Qian, Mohsin Pasha, Yuhan Wang, Jiayi Li, Yuzhe Liu, Saier Liu, Xiao Xue, Min Qiu, Zihao Zhong, Minjing Shang, Jie Zheng, Zhigang Lin, Yuanhai Su","doi":"10.1002/aic.18693","DOIUrl":"10.1002/aic.18693","url":null,"abstract":"Photobromination reaction of oxime ether (OE) to brominated oxime ether (BOE) is an important process for the synthesis of trifloxystrobin in the fungicide industry. Herein, continuous synthesis of BOE in photomicroreactors was performed. Initially, an investigation was carried out to study the effects of various parameters, including mixing performance, molar ratios, solvents, incident photon flux, and temperature, on the photobromination process. Moreover, a kinetic model was established, and the activation energies for the main and side reactions were determined. The relationship between the reaction rate constant and light flux was illuminated. Transition states and energy changes in the bromination process were analyzed using density functional theory calculation. Remarkably, an 83.1% yield of BOE was achieved in the photomicroreactor and the required reaction time was reduced to approximately 1/10 of the batch reactor. This work was of crucial theoretical significance and practical value for better understanding of photobromination processes and parameter optimization.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"71 3","pages":""},"PeriodicalIF":3.5,"publicationDate":"2024-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142797389","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

Enhanced resistance to poisoning of Pd in alkynes semi-hydrogenation by metal–ligand electronic interactions 金属-配体电子相互作用增强炔烃半氢化对Pd中毒的抗性

IF 3.5 3区工程技术

AIChE Journal Pub Date : 2024-12-08 DOI: 10.1002/aic.18687

Zhongzhe Wei, Guanglu Dong, Long Zhao, Songtao Huang, Molin Xia, Wei Huang, Ming Jiang, Zhixiang Yang, Zihao Yao, Jianfeng Li, Jianguo Wang

{"title":"Enhanced resistance to poisoning of Pd in alkynes semi-hydrogenation by metal–ligand electronic interactions","authors":"Zhongzhe Wei, Guanglu Dong, Long Zhao, Songtao Huang, Molin Xia, Wei Huang, Ming Jiang, Zhixiang Yang, Zihao Yao, Jianfeng Li, Jianguo Wang","doi":"10.1002/aic.18687","DOIUrl":"10.1002/aic.18687","url":null,"abstract":"Given that the retention of nitrogen readily renders active site poisoning, designing versatile catalysts characterized by notable selectivity and even resistance to poisoning for alkyne semi-hydrogenation under nitrogen-containing conditions is considerably challenging. In this article, oxanilide-decorated Pd/C (Pd/C-oxa) catalyst is facilely synthesized by leveraging impregnation-coordination, which exhibit remarkable performance in the semi-hydrogenation of nitrogen-containing alkynes, with ultrahigh turnover frequency (TOF) of 15,831 h−1 and selectivity of 97.2%. Strikingly, it still sustains TOF of 12,137 h−1 in a sulfur-containing system, demonstrating distinguished tolerance to sulfur. Comprehensive studies corroborate that oxanilide tunes the electron density of Pd by constructing metal–ligand electronic interactions, facilitating hydrogen activation. Simultaneously, the reaction microenvironment is optimized, which effectively promotes the desorption of nitrogen-containing olefins and attenuates the aggregation of nitrogen on the Pd surface. This strategy is universal and holds promising industrial applications, making it appropriate for use in commercial Pd/C catalysts as well.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"71 3","pages":""},"PeriodicalIF":3.5,"publicationDate":"2024-12-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142793396","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