ACS Engineering AuPub Date : 2025-07-11DOI: 10.1021/acsengineeringau.5c00034
Prachi Upadhyay, Artina Deka and Sankar Chakma*,
{"title":"Unlocking Efficient Electrochemical Urea Oxidation and Understanding Mechanism Insights of Co-Doped NiS","authors":"Prachi Upadhyay, Artina Deka and Sankar Chakma*, ","doi":"10.1021/acsengineeringau.5c00034","DOIUrl":"https://doi.org/10.1021/acsengineeringau.5c00034","url":null,"abstract":"<p >Urea electrooxidation serves as the core of urea-based fuel cells, urea electrolysis for energy generation, and urea-based wastewater treatment for environmental applications. This study emphasizes the development of electrocatalysts made from nickel–cobalt bimetallic sulfide, synthesized through an ultrasonic-assisted hydrothermal synthesis method, focusing on their capacity to oxidize urea under alkaline conditions. The objective was to reduce the onset potential for this reaction. These nickel–cobalt bimetallic sulfide catalysts were characterized by using various techniques, including X-ray diffraction analysis (XRD), scanning electron microscopy (SEM), cyclic voltammetry (CV), and electrochemical impedance spectroscopy (EIS). A notable decrease in overpotential was observed: 70 mV for Ni<sub>0.75</sub>Co<sub>0.25</sub>S and 130 mV for Ni<sub>0.50</sub>Co<sub>0.50</sub>S, compared to a Ni<sub>1</sub>Co<sub>0</sub>S electrode. Furthermore, the XPS analysis indicates that the ratio of Ni<sup>3+</sup>/Ni<sup>2+</sup> is higher for Ni<sub>0.75</sub>Co<sub>0.25</sub>S than for other combinations, with Ni<sup>3+</sup> acting as the primary active center for urea electrooxidation. This reduction in the onset potential for urea oxidation and the increase in Ni<sup>3+</sup> on the nickel–cobalt bimetallic sulfide electrodes reveal significant potential for future applications in urea electrooxidation.</p>","PeriodicalId":29804,"journal":{"name":"ACS Engineering Au","volume":"5 4","pages":"450–467"},"PeriodicalIF":5.1,"publicationDate":"2025-07-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acsengineeringau.5c00034","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144862848","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Engineering AuPub Date : 2025-07-10DOI: 10.1021/acsengineeringau.5c00046
Squire J. Booker, Stephanie L. Brock, Xiangdong Li, Géraldine Masson, Sébastien Perrier, Vivek V. Ranade, Raymond E. Schaak, Gemma C. Solomon and Shelley D. Minteer*,
{"title":"Introducing the Tutorial Manuscript Type at the ACS Au Community Journals","authors":"Squire J. Booker, Stephanie L. Brock, Xiangdong Li, Géraldine Masson, Sébastien Perrier, Vivek V. Ranade, Raymond E. Schaak, Gemma C. Solomon and Shelley D. Minteer*, ","doi":"10.1021/acsengineeringau.5c00046","DOIUrl":"https://doi.org/10.1021/acsengineeringau.5c00046","url":null,"abstract":"","PeriodicalId":29804,"journal":{"name":"ACS Engineering Au","volume":"5 4","pages":"312–313"},"PeriodicalIF":5.1,"publicationDate":"2025-07-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acsengineeringau.5c00046","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144862842","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Engineering AuPub Date : 2025-07-09DOI: 10.1021/acsengineeringau.5c00033
Phebe Lemaire, Arno de Reviere, Dhanjay Sharma, Valérie Ruaux, Jaouad Al Atrach, Valentin Valtchev, Joris Thybaut, Maarten Sabbe and An Verberckmoes*,
{"title":"The Influence of Mesopore Architecture in Hierarchical H-ZSM-5 on n-Butanol Dehydration","authors":"Phebe Lemaire, Arno de Reviere, Dhanjay Sharma, Valérie Ruaux, Jaouad Al Atrach, Valentin Valtchev, Joris Thybaut, Maarten Sabbe and An Verberckmoes*, ","doi":"10.1021/acsengineeringau.5c00033","DOIUrl":"https://doi.org/10.1021/acsengineeringau.5c00033","url":null,"abstract":"<p >Zeolites are among the most widely employed catalysts in the (petro-)chemical industry. However, due to their elaborate microporous network, they are prone to diffusion limitations and deactivation. Several modification methods have been proposed to overcome these limitations, each exhibiting their benefits. In this work, two of the most promising strategies were combined, i.e., limiting the length of one of the crystal axes during synthesis to achieve a platelike morphology and introducing mesoporosity, creating a hierarchical platelike H-ZSM-5. The platelike morphology was obtained by adding urea as a growth modifier to the synthesis mixture, and mesopores were introduced in the platelike H-ZSM-5 through etching with a NaOH/TPAOH mixture. As a benchmark, the same etching procedure was applied to a commercial ZSM-5 counterpart. These materials were tested in the n-butanol dehydration, where the platelike morphology exhibited an improved catalytic performance, significantly increasing the activity per acid site and stability, and slightly increasing the selectivity toward the butenes. The generation of mesopores in commercial ZSM-5 also increased the activity per acid site but reduced the catalyst’s stability, likely due to an increased amount of Lewis acid sites upon etching. When applying the same modification method to the platelike H-ZSM-5, much larger mesopores and some macropores were observed. These further increased the stability of the catalyst but barely affected the activity per acid site, presumably due to the already optimized catalytic performance of the platelike H-ZSM-5.</p>","PeriodicalId":29804,"journal":{"name":"ACS Engineering Au","volume":"5 4","pages":"434–449"},"PeriodicalIF":5.1,"publicationDate":"2025-07-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acsengineeringau.5c00033","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144863137","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Engineering AuPub Date : 2025-07-03DOI: 10.1021/acsengineeringau.5c00030
Tzu-Hung Wen, Wei-Lun Huang, Po-Yang Peng, Ying-Rui Lu, Chi-Liang Chen, Bryan R. Goldsmith and Yu-Chuan Lin*,
{"title":"Bayesian Optimization-Guided Design of Silica-Supported Nickel Catalysts from Nickel Phyllosilicates","authors":"Tzu-Hung Wen, Wei-Lun Huang, Po-Yang Peng, Ying-Rui Lu, Chi-Liang Chen, Bryan R. Goldsmith and Yu-Chuan Lin*, ","doi":"10.1021/acsengineeringau.5c00030","DOIUrl":"https://doi.org/10.1021/acsengineeringau.5c00030","url":null,"abstract":"<p >Here, we report a Bayesian optimization (BO)-guided approach to optimize Ni/SiO<sub>2</sub> catalyst synthesis from the reduction of nickel phyllosilicate (rNiPS). Key synthesis parameters─calcination temperature, calcination time, reduction temperature, and reduction time─were tuned to maximize the concentration of exsolved Ni<sup><i>x</i>+</sup> species and Ni<sup>0</sup> nanoparticles, which are active sites for levulinic acid (LA) hydrogenation to γ-valerolactone (GVL). Using 15 initial samples of differently synthesized rNiPS catalysts (rNiPS-1 to rNiPS-15) to initiate the BO with Gaussian process regression, we rapidly identified synthesis conditions after three iterations, which increase the combined concentrations of Ni<sup><i>x</i>+</sup> (<i>x</i> = ∼1.66) and Ni<sup>0</sup>/10 by ∼14% (rNiPS-18) compared to the benchmark. The optimized catalyst’s physicochemical properties, including porosity, crystallinity, reducibility, surface acidity, and local Ni geometry, were analyzed, revealing higher Ni<sup><i>x</i>+</sup> and lower Ni<sup>0</sup> concentrations than the benchmark catalyst. Additionally, the turnover frequency of rNiPS-18 for LA hydrogenation to GVL increased nearly 50% compared to that of the benchmark, underscoring BO’s effectiveness in designing Ni catalysts enriched with Ni<sup><i>x</i>+</sup> and Ni<sup>0</sup>.</p>","PeriodicalId":29804,"journal":{"name":"ACS Engineering Au","volume":"5 4","pages":"425–433"},"PeriodicalIF":5.1,"publicationDate":"2025-07-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acsengineeringau.5c00030","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144863063","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Engineering AuPub Date : 2025-06-18DOI: 10.1021/acsengineeringau.5c00031
Muhammad Usman, and , Tetsuya Yamada*,
{"title":"Methanol Reforming for Hydrogen Production: Advances in Catalysts, Nanomaterials, Reactor Design, and Fuel Cell Integration","authors":"Muhammad Usman, and , Tetsuya Yamada*, ","doi":"10.1021/acsengineeringau.5c00031","DOIUrl":"https://doi.org/10.1021/acsengineeringau.5c00031","url":null,"abstract":"<p >Methanol reforming has emerged as a leading pathway for on-demand hydrogen production, particularly for applications in portable power and fuel cells. This review offers a comprehensive analysis of methanol steam reforming (MSR), partial oxidation (POX), autothermal reforming (ATR), and recent integration strategies with renewable systems and fuel cells. Emphasis is placed on catalyst design, reaction mechanisms, reactors, operational parameters, and recent nanostructured catalyst innovations, such as single-atom catalysts (SACs), bimetallic, carbon nanotubes, perovskites, and alloy nanomaterials. This review critically evaluates recent progress, highlighting how tailored catalyst morphologies, metal–support interactions, and synthesis methods translate into enhanced methanol conversion, H<sub>2</sub> selectivity, and CO suppression. Notably, low-temperature SACs and Zn-modified bimetallic systems exhibit remarkable performance metrics, pointing toward viable pathways for clean hydrogen production. Furthermore, emerging approaches like plasma-assisted dry reforming and chemical looping integration present promising solutions for CO<sub>2</sub> utilization. Recent applications of artificial intelligence (AI) in catalyst screening and reaction modeling also show potential to accelerate the discovery of high-efficiency systems. By synthesizing these findings and identifying the gaps in current research, this review outlines future directions for scalable, low-emission methanol reforming technologies, aiming to support the global transition toward a hydrogen-based energy economy.</p>","PeriodicalId":29804,"journal":{"name":"ACS Engineering Au","volume":"5 4","pages":"314–346"},"PeriodicalIF":5.1,"publicationDate":"2025-06-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acsengineeringau.5c00031","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144863055","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Balachandran Subramanian*, K. Jeeva Jothi, Mohamedazeem M. Mohideen, R. Karthikeyan, A. Santhana Krishna Kumar*, Ganeshraja Ayyakannu Sundaram, K. Thirumalai, Munirah D. Albaqami, Saikh Mohammad and M. Swaminathan*,
{"title":"","authors":"Balachandran Subramanian*, K. Jeeva Jothi, Mohamedazeem M. Mohideen, R. Karthikeyan, A. Santhana Krishna Kumar*, Ganeshraja Ayyakannu Sundaram, K. Thirumalai, Munirah D. Albaqami, Saikh Mohammad and M. Swaminathan*, ","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":29804,"journal":{"name":"ACS Engineering Au","volume":"5 3","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":4.3,"publicationDate":"2025-06-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acsengineeringau.5c00015","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144429466","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}