{"title":"Discharge reactor for fabricating efficient supported metal catalysts at room temperature in the absence of H2","authors":"Peng Liu, Xin-Yu Meng, Xujun Wang, Yiyi Zhao, Yu-Long Men, Yun-Xiang Pan","doi":"10.1002/aic.18669","DOIUrl":"https://doi.org/10.1002/aic.18669","url":null,"abstract":"Supported metal catalysts have been widely applied and commonly fabricated through the H<sub>2</sub> reduction process. Herein, we develop a H<sub>2</sub>-free room-temperature discharge-driven reduction (RT-DR) reactor for fabricating supported metal catalysts at room temperature without H<sub>2</sub>. By RT-DR reactor, a catalyst with pseudo-boehmite (PB) as support (CdS/Pt/PB) is fabricated. In visible-light-driven photocatalytic H<sub>2</sub>O splitting to H<sub>2</sub>, CdS/Pt/PB shows a H<sub>2</sub> evolution rate of 1132 μmol h<sup>−1</sup>, which is greatly enhanced than that on catalyst prepared by traditional H<sub>2</sub>-reduction (633 μmol h<sup>−1</sup>). RT-DR reactor is also used to prepare a catalyst with low sodium PB (LSPB) as support (CdS/Pt/LSPB). In visible-light-driven photocatalytic H<sub>2</sub>O splitting to H<sub>2</sub>, CdS/Pt/LSPB shows a H<sub>2</sub> evolution rate of 2554 μmol h<sup>−1</sup>, which is 2.5 times higher than that on catalyst prepared by traditional H<sub>2</sub>-reduction (1029 μmol h<sup>−1</sup>). Thus, RT-DR reactor has high efficiency and universality in preparing catalysts, thus offering a great potential for commercialization.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"74 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2024-11-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142756269","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}
AIChE JournalPub Date : 2024-11-29DOI: 10.1002/aic.18670
Zhenbin Gu, Jinkun Tan, Haoli Zhou, Zhengkun Liu, Lin Ge, Guangru Zhang, Wanqin Jin
{"title":"High H2 permeability in F-doped BaZr0.7Ce0.2Y0.1O3−δ perovskite membranes via thermodynamic controlled sintering","authors":"Zhenbin Gu, Jinkun Tan, Haoli Zhou, Zhengkun Liu, Lin Ge, Guangru Zhang, Wanqin Jin","doi":"10.1002/aic.18670","DOIUrl":"https://doi.org/10.1002/aic.18670","url":null,"abstract":"A raw hydrogen mixture frequently results in a reduction in conversion efficiency and the generation of undesired by-products. The application of advanced membrane technology has the potential to offer an economically viable solution for the recovery of hydrogen from such mixtures. BaZr<sub>1−x−y</sub>Ce<sub>x</sub>Y<sub>y</sub>O<sub>3−δ</sub> is increasingly regarded as an optimal perovskite hydrogen permeable membrane. Nevertheless, the main drawback to its use in a larger scale is the extremely low hydrogen permeability and stability. An original perovskite material is proposed in this study, BaZr<sub>0.7</sub>Ce<sub>0.2</sub>Y<sub>0.1</sub>O<sub>3−δ</sub>-F<sub>x</sub>. A thermodynamic-controlled sintering strategy (TCS) has been employed to inhibit the evaporation of metals from ceramic solids. The TCS directly caused the hydrogen permeation flux to reach 1.07 ml·min<sup>−1</sup> cm<sup>−2</sup>, representing a fourfold improvement. Furthermore, F-doping demonstrated enhanced performance at low and medium temperatures. The aforementioned successful strategy provides an effective path for the tailoring of perovskite materials and promotes its application for the industrial-scale separation of hydrogen.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"1 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2024-11-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142756388","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}
{"title":"Stabilization of cuσ+ via strong Cu-O-Si interface for efficient electrocatalytic acetylene semi-hydrogenation","authors":"Xiaoli Jiang, Wangxin Ge, Yu Fan, Xuedi Sheng, Hongliang Jiang, Chunzhong Li","doi":"10.1002/aic.18663","DOIUrl":"https://doi.org/10.1002/aic.18663","url":null,"abstract":"The development of a high-performance electrocatalytic acetylene semi-hydrogenation catalyst is the key to the selective removal of acetylene from industrial ethylene gas and non-oil route to ethylene production. However, it is still hampered by the deactivation of the catalyst and hydrogen evolution interference. Here, we proposed an interface engineering strategy involving the Cu and cupric oxide nanoparticles dispersed on amorphous SiO<sub>2</sub> (Cu/CuO<sub><i>x</i></sub>/SiO<sub>2</sub>) by a simple stöber method. x-ray photoelectron spectroscopy demonstrated the strong interfacial interaction between cupric oxide nanoparticles and SiO<sub>2</sub>. The formed Cu-O-Si interface stabilized the Cu<sup>σ+</sup> at high reduction potentials, thus improving the activity and stability of the acetylene reduction reaction, as confirmed by in situ Raman spectroscopy. Consequently, the electrochemical test results showed that at 0.5 M KHCO<sub>3</sub>, the maximum Faraday efficiency (FE) of ethylene on the optimized Cu/CuO<sub><i>x</i></sub>/SiO<sub>2</sub> reached 96%. And ethylene FE remains above 85% at −100 mA cm<sup>−2</sup> for 40 h.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"196 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2024-11-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142742796","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}
{"title":"A highly integrated ceramic membrane-based reactor for intensifying the biomass gasification to clean syngas","authors":"Wei Wei, Qiaoqiao Zhou, Ajing Ding, Shuncheng Li, Feng Zeng, Xuerui Wang, Chong Tian, Zhaoxiang Zhong, Huanhao Chen, Xuehong Gu","doi":"10.1002/aic.18647","DOIUrl":"https://doi.org/10.1002/aic.18647","url":null,"abstract":"Biomass gasification for syngas production is a key operating unit in the biomass utilization process. However, its overall efficiency and stability are often restricted by the presence of complex impurities, including particulate matters (PMs) and tars. In this study, a highly integrated ceramic membrane-based reactor was developed for high-temperature syngas cleaning, enabling the efficient <i>in situ</i> removal of PMs and tars from bio-vapors produced by biomass gasification. Specifically, a silicon carbide (SiC) membrane could separate PMs from biomass volatiles <i>in situ</i>, while a structured Ni<sub>15</sub>La<sub>5</sub>/S1-SiC catalyst (nickel and lanthanum-laden silicalite-1 zeolite supported on SiC foam) facilitated the catalytic reforming of tars. Compared to other control reactors (i.e., those containing either a membrane or catalyst alone), the integrated reactor showed synergistic intensification in producing clean syngas from biomass gasification, achieving PM and tar removal efficiencies of up to ~97% and ~90%, and exhibited excellent stability in five-cycle evaluations at 800°C.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"38 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2024-11-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142713043","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}
{"title":"Boosting electrocatalytic alcohol oxidation: Efficient d–π interaction with modified TEMPO and bioinspired structure","authors":"Ying Chen, Shibin Wang, Zaixiang Xu, Yuhang Wang, Jiahui He, Kai Li, Jieyu Wang, Lihao Liu, Linhan Ren, Suiqin Li, Zhengbin Zhang, Xing Zhong, Jianguo Wang","doi":"10.1002/aic.18662","DOIUrl":"https://doi.org/10.1002/aic.18662","url":null,"abstract":"Aminoxyl radicals electrocatalysis presents a sustainable method for oxidizing alcohols into high-value products. Nonetheless, the requirement for high doses of aminoxyl radicals diminishes product purity and economic viability. This study synthesized methylimidazole-functionalized 4-acetylamino-2,2,6,6-tetramethylpiperidine-N-oxyl derivative (MIAcNH-TEMPO) with a strongly electron-withdrawing imidazole group and combined it with bioinspired nickel-supported carbonaceous octopus tentacles for effective electrooxidation of alcohols, achieving high current density of 200 mA cm<sup>−2</sup>, selectivity of 99%, and turnover frequency of 26,490 h<sup>−1</sup>. In situ experiments and theoretical calculations indicated that the synergistic effect of Ni-3d<sub><i>xz</i></sub> orbitals on the tentacle surface interacting with the π orbitals of MIAcNH-TEMPO creates a strong d–π interaction, which effectively facilitating the creation of a locally intermediate-enriched microenvironment, decreased the required quantity of aminoxyl radicals. Moreover, the high aqueous solubility of MIAcNH-TEMPO reduces the difficulty of separation process. Scale-up experiments conducted in a continuous flow electrolyzer showcased the potential of this strategy for practical applications.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"38 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2024-11-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142713044","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}
AIChE JournalPub Date : 2024-11-26DOI: 10.1002/aic.18642
Marco Avendano, Qiang Fu, Jianpei Lao, Sankar Nair, Matthew J. Realff
{"title":"Simultaneous optimization of simulated moving bed adsorption and distillation for 2,3-butanediol recovery","authors":"Marco Avendano, Qiang Fu, Jianpei Lao, Sankar Nair, Matthew J. Realff","doi":"10.1002/aic.18642","DOIUrl":"https://doi.org/10.1002/aic.18642","url":null,"abstract":"A combined simulated moving bed (SMB) and distillation separation scheme is developed to recover 2,3-butanediol (BDO) from a dilute fermentation broth. The scheme was integrated into a lignocellulosic biorefinery that produces hydrocarbon fuels from corn stover with BDO as an intermediate. BDO recovery is one of the most challenging processes in this biorefinery; and given the high associated energy duties, direct distillation is considered cost-prohibitive. An alternative separation is SMB adsorption in nanoporous materials, which can reject 90% of the water and reduce subsequent distillation costs. Rigorous models were used to optimize the SMB and distillation simultaneously. The separation can be added to the biorefinery while keeping the projected minimum fuel selling price (MFSP) below $0.66 USD (US dollars) per liter gasoline-equivalent ($2.50/GGE, gallon gasoline equivalent). Finally, sensitivity analyses were conducted to assess the effects of cost and lifetime of the adsorbent, titer concentration, and BDO purity.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"8 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2024-11-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142713042","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}
AIChE JournalPub Date : 2024-11-26DOI: 10.1002/aic.18666
Ying Tian, Changqing He, Xincheng Zhang, Lin He, Zhenghe Xu, Hong Sui, Xingang Li
{"title":"Doping Si/O to enhance interfacial occupancy of demulsifiers for low-carbon breaking of water-in-heavy oil emulsions","authors":"Ying Tian, Changqing He, Xincheng Zhang, Lin He, Zhenghe Xu, Hong Sui, Xingang Li","doi":"10.1002/aic.18666","DOIUrl":"https://doi.org/10.1002/aic.18666","url":null,"abstract":"Separating water-in-heavy oil (W/HO) emulsions at low (room) temperature is challenging when exploiting heavy oil. We propose an adaptable strategy for constructing Si/O-doped demulsifiers. A nonionic demulsifier (APBMP) has been synthesized based on polysiloxane modified by allyl polyether and butyl acrylate. APBMP achieves 95.97% dehydration within 5 min for W/HO emulsions at 288.15 K and complete dehydration in 15 min at 323.15 K. Mechanistic studies found that doping Si/O into the demulsifier molecules increases the number of hydrogen bond sites, which enables the demulsifiers to quickly disperse natural stabilizers (e.g., asphaltenes) and replace them at the oil–water interfacial film. The demulsifiers prefer to occupy the interfacial sites rather than dissolve into the bulk oil or water phases. Driven by hydrogen-bond-dominated noncovalent interactions, the oil–water interfacial film is softened, reconstructed, and broken. These findings provide insights into developing novel materials for oil–water separations in a low-carbon way.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"12 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2024-11-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142742801","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}
{"title":"Incorporation of Lewis basic sites into Zn-pyrazolate frameworks for efficient methane/nitrogen separation","authors":"Jiaqi Liu, Jiafeng Miao, Lulu Ma, Jinping Li, Jing Li, Hao Wang","doi":"10.1002/aic.18656","DOIUrl":"https://doi.org/10.1002/aic.18656","url":null,"abstract":"The separation of methane (CH<sub>4</sub>) and nitrogen (N<sub>2</sub>) in coalbed methane (CBM) is a crucial process to produce methane as a clean energy source. Given the similar physicochemical properties of the two gases, efficient adsorptive separation of CH<sub>4</sub> and N<sub>2</sub> has stringent requirements on the pore chemistry and geometry of the adsorbents. In this study, we report two Zn-pyrazolates frameworks, HIAM-213 and HIAM-214, which possess Lewis basic sites that exhibit precise recognition of CH<sub>4</sub> over N<sub>2</sub>. The capability of these compounds in extracting CH<sub>4</sub> from binary CH<sub>4</sub>/N<sub>2</sub> mixtures has been confirmed through column breakthrough measurements, demonstrating a high recovery rate under mild regeneration conditions. Grand canonical Monte Carlo simulations and in situ Fourier transform infrared spectroscopy experiments provide insights into the selective adsorption mechanism by revealing stronger interactions between CH<sub>4</sub> and Lewis acid sites.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"37 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2024-11-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142756397","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}
AIChE JournalPub Date : 2024-11-25DOI: 10.1002/aic.18635
Landon Schofield, Benjamin Paren, Ruaridh Macdonald, Yang Shao-Horn, Dharik Mallapragada
{"title":"Dynamic optimization of proton exchange membrane water electrolyzers considering usage-based degradation","authors":"Landon Schofield, Benjamin Paren, Ruaridh Macdonald, Yang Shao-Horn, Dharik Mallapragada","doi":"10.1002/aic.18635","DOIUrl":"10.1002/aic.18635","url":null,"abstract":"<p>We present a techno-economic optimization model for the design and dynamic operation of proton exchange membrane (PEM) electrolyzers, for enabling cost-effective hydrogen production. This model integrates a 0-D model of the electrolyzer stack, process-wide mass and energy balances, operational constraints, and an empirical relation to characterize degradation as a function of operating current density. Utilizing a decomposition-based solution approach, the model predicts optimal electrolyzer size, operation, and necessary hydrogen storage to satisfy hydrogen demand across various technology and electricity price scenarios. Analysis for 2022 electricity prices and technology costs shows that including use-dependent degradation raises the levelized cost of hydrogen (LCOH) from $4.56/kg to $6.60/kg and increases frequency of stack replacement (2 vs. 7 years). However, by 2030, we anticipate a significant reduction in LCOH to $2.50/kg due to lower capital expenses, leading to longer stack lifetimes and less hydrogen storage. The proposed modeling framework is adaptable to study other electrochemical systems relevant for decarbonization.</p>","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"71 1","pages":""},"PeriodicalIF":3.5,"publicationDate":"2024-11-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142696708","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}
{"title":"Unlocking electrodialysis efficiency with spacer mesh geometry and material conductivity via finite element analysis","authors":"Yuyang Yao, Junjie Mu, Yueyue Lu, Edison Huixiang Ang, Jiangnan Shen","doi":"10.1002/aic.18653","DOIUrl":"https://doi.org/10.1002/aic.18653","url":null,"abstract":"Spacer meshes in electrodialysis (ED) play a crucial role in influencing fluid and electric field distributions during mass transfer. This study employed finite element analysis using real-world parameters to explore how spacer mesh geometry and material affect mass transport. Comparisons among different wire mesh configurations revealed increased fluid velocity near mesh wires and reduced electric field intensity nearby, enhancing overall transport efficiency. Increasing mesh count or wire diameter notably improves transport, with optimal results achieved when wire orientation aligns with fluid flow. Additionally, the study showed that spacer mesh conductivity significantly influences ED transport, particularly when it exceeds the conductivity of the solution. These findings advance the design and application of spacer meshes, offering valuable insights for future developments in ED technology.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"34 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2024-11-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142713045","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}