Energy & FuelsPub Date : 2025-05-19DOI: 10.1021/acs.energyfuels.4c0524610.1021/acs.energyfuels.4c05246
Xinyi Zhou, Weisong Yang, Chenyu Wu, Shengjuan Li and Lei Li*,
{"title":"Zinc-Ion Hybrid Supercapacitors: A Review on Electrode Materials, Electrolytes, and Diaphragms to Inhibit Zinc Dendrite Growth","authors":"Xinyi Zhou, Weisong Yang, Chenyu Wu, Shengjuan Li and Lei Li*, ","doi":"10.1021/acs.energyfuels.4c0524610.1021/acs.energyfuels.4c05246","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.4c05246https://doi.org/10.1021/acs.energyfuels.4c05246","url":null,"abstract":"<p >Zinc-ion hybrid supercapacitors (ZHSCs) combine the high energy of zinc-ion batteries with supercapacitors’ long life and high power density. Therefore, they are considered promising candidates for next-generation high-performance energy storage systems. However, zinc dendrite growth, which can puncture the diaphragm, leading to short circuits and capacity degradation, is a current challenge for ZHSCs. This review summarizes the research progress of ZHSCs in cathodes (including carbon-based materials, transition metal oxides, MXenes, and conductive polymers), anodes, electrolytes, and diaphragms. It also describes the effects of electrode material structure, electrolyte composition, and diaphragm structure on the growth of zinc dendrites to offer methods for enhancing the performance of ZHSCs.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"39 21","pages":"9641–9667 9641–9667"},"PeriodicalIF":5.2,"publicationDate":"2025-05-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144166051","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 & FuelsPub Date : 2025-05-18DOI: 10.1021/acs.energyfuels.5c0116910.1021/acs.energyfuels.5c01169
Tao Liu, Peng Wu, Qingyong Lu, Xin Lv, Shi Shen, Huiyong Liang and Yanghui Li*,
{"title":"Elastic–Plastic Behavior of Hydrate-Bearing Sediments of the South China Sea under Triaxial Cyclic Loading","authors":"Tao Liu, Peng Wu, Qingyong Lu, Xin Lv, Shi Shen, Huiyong Liang and Yanghui Li*, ","doi":"10.1021/acs.energyfuels.5c0116910.1021/acs.energyfuels.5c01169","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.5c01169https://doi.org/10.1021/acs.energyfuels.5c01169","url":null,"abstract":"<p >The comprehensive evaluation of the mechanical behavior stability of hydrate reservoirs is critical for ensuring the success of upcoming industrial trial production. However, potential cyclic loading conditions, such as those caused by periodic vibrations from pile foundations, hydraulic fracturing, and similar activities, are often overlooked. In this study, the clay-silty sediment from the South China Sea was remolded and subjected to drained cyclic triaxial experiments under varying saturation levels (0–45%) and effective confining pressures (1–3 MPa). The following conclusions were drawn: the hydrate sediments show a significant elastic–plastic behavior during cyclic loading and unloading, which leads to energy dissipation; their volumetric strain shows volumetric shrinkage during loading and volumetric expansion during unloading; their Poisson’s ratios change with hydrate saturation and the effective confining pressure, with fluctuations in the range of 0.1 to 0.3; and it is also found that the dependence of the elastic modulus of the hydrate sediments on the axial stress exhibited a linear relationship. This study provides valuable data to support the stability analysis of gas hydrate reservoirs.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"39 21","pages":"9818–9827 9818–9827"},"PeriodicalIF":5.2,"publicationDate":"2025-05-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144165982","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 & FuelsPub Date : 2025-05-17DOI: 10.1021/acs.energyfuels.5c0130810.1021/acs.energyfuels.5c01308
Valentina Sierra-Jimenez, Théo Voellinger, Vincent Carré, Farid Chejne, Sébastien Schramm, Frédéric Aubriet and Manuel Garcia-Perez*,
{"title":"Exploring Cellulose Fast Pyrolysis Secondary Reactions Through Reactive Molecular Dynamics and Direct Insertion Probe Fourier Transform Ion Cyclotron Resonance Mass Spectrometry","authors":"Valentina Sierra-Jimenez, Théo Voellinger, Vincent Carré, Farid Chejne, Sébastien Schramm, Frédéric Aubriet and Manuel Garcia-Perez*, ","doi":"10.1021/acs.energyfuels.5c0130810.1021/acs.energyfuels.5c01308","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.5c01308https://doi.org/10.1021/acs.energyfuels.5c01308","url":null,"abstract":"<p >Although extensive literature exists on the depolymerization, fragmentation, and dehydration reactions occurring during cellulose pyrolysis, little is known about the secondary reactions involving dehydrated and fragmented oligomeric molecules that lead to the formation of highly modified oligomeric products in bio-oils and char. These secondary reactions are of significant practical importance. The highly dehydrated and modified dimers and trimers present in bio-oils are believed to act as coke precursors during hydrotreatment, while the larger oligomeric products contribute to char formation during pyrolysis. To bridge this knowledge gap, this study employs molecular dynamics simulations using the reactive force field (ReaxFF) to investigate the secondary reactions of dehydrated cellulose oligomers and the mechanisms driving heavy fraction formation. Postsimulation analysis identified over 400 reactions, proposed multiple reaction networks, and revealed key intermediates. To validate the modeling strategy, theoretical predictions were compared with experimental data obtained via direct insertion probe Fourier transform ion cyclotron resonance mass spectrometry (DIP FT-ICR MS) in the 87–1000 Da mass range. Probability distribution functions and molecular weight distribution analysis showed a 77% overlap between ReaxFF predictions and DIP FT-ICR MS data, confirming the reliability of the modeling strategy in forecasting fast pyrolysis behavior. Further validation was achieved through a van Krevelen diagram, which demonstrated that char fragments derived from ReaxFF simulations closely aligned with experimental data for cellulose char obtained at 400 °C. By integrating computational and experimental approaches, this study provides new insights into the secondary reactions of cellulose oligomers, highlights the role of key intermediates and water removal in these processes, and offers new opportunities for advancing selective biomass conversion technologies.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"39 21","pages":"9860–9873 9860–9873"},"PeriodicalIF":5.2,"publicationDate":"2025-05-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144165962","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 & FuelsPub Date : 2025-05-16DOI: 10.1021/acs.energyfuels.5c0174410.1021/acs.energyfuels.5c01744
Malcolm A. Kelland*, and , Janronel Pomicpic,
{"title":"Key Structural Features for an Effective Kinetic Hydrate Inhibitor─You Need Them All!","authors":"Malcolm A. Kelland*, and , Janronel Pomicpic, ","doi":"10.1021/acs.energyfuels.5c0174410.1021/acs.energyfuels.5c01744","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.5c01744https://doi.org/10.1021/acs.energyfuels.5c01744","url":null,"abstract":"<p >Kinetic gas hydrate inhibitor (KHI) liquid formulations have been used since the mid-1990s as a method to prevent gas hydrate formation in oil and gas production flow lines. All commercial KHIs contain one or more polymers as the key active ingredient. Among the commercial homopolymers, poly(<i>N</i>-vinylpyrrolidone) (PVP) is considered a mild KHI (low performance), whereas poly(<i>N</i>-vinylcaprolactam) (PVCap) or poly(<i>N</i>-isopropylmethacrylamide) (PNIPMAM) are powerful KHIs (high performance). Our contention is that KHI formulations only give high performance if they contain one or more water-soluble molecules with a high density of multiple amphiphilic groups with the correct size hydrophobic groups adjacent to strong hydrogen-bonding groups. This often means oligomers or polymers (as well as copolymers), but other molecules with a high density of the correct multiple amphiphilic groups can also be used. Blends of such molecules, or addition of certain molecules that do not conform to the theory, can be added to boost the performance. Here we review past work related to this claim and present experimental results on some molecules recently reported to be active KHIs, but which fall outside our structural definition of what makes a good KHI. These molecules all gave very poor KHI performance in our steel rocking cell equipment using either methane or a natural gas mixture in slow (1.0 °C/h) constant cooling tests when compared to classic KHIs such as PVCap. They include safranine O, several amino acids, <span>l</span>-ascorbic acid, alanine-glycine dipeptide, 18-crown-6 ether, hydroxyethylcellulose, pectin, carboxymethylguar, iota- and lamba-carrageenans, and poly(vinyl alcohol) (PVA) plus several more hydrophobically modified PVA derivatives. Finally, based on 34 years of KHI experience, we give some advice to new KHI researchers.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"39 21","pages":"9802–9817 9802–9817"},"PeriodicalIF":5.2,"publicationDate":"2025-05-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.energyfuels.5c01744","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144165845","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}
Energy & FuelsPub Date : 2025-05-16DOI: 10.1021/acs.energyfuels.5c0062510.1021/acs.energyfuels.5c00625
Mingqiang Chen*, Yupei Li, Yishuang Wang*, Defang Liang, Chang Li, Haosheng Xin and Jun Wang,
{"title":"Catalytic Depolymerization of Lignin over B–Ti-Modified Diatomite-Supported Nickel Phosphide Catalysts Using Formic Acid-Assisted Aqueous-Phase Glycerol","authors":"Mingqiang Chen*, Yupei Li, Yishuang Wang*, Defang Liang, Chang Li, Haosheng Xin and Jun Wang, ","doi":"10.1021/acs.energyfuels.5c0062510.1021/acs.energyfuels.5c00625","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.5c00625https://doi.org/10.1021/acs.energyfuels.5c00625","url":null,"abstract":"<p >Catalytic depolymerization of lignin (CDL) is a prospective technology for the efficient utilization of biomass. In this paper, novel B–Ti-modified diatomite-supported nickel phosphide catalysts (<i>x</i>NiP/BTD) were prepared to depolymerize lignin in a unique formic acid-assisted aqueous-phase glycerol medium. Under optimal conditions, 4NiP/BTD exhibited 100% lignin conversion and 95.4% lignin oil (LO) yield, in which the yield of petroleum ether (PE)-soluble product reached 20.6%. Based on the characterization results, the superior performance of 4NiP/BTD for CDL was attributed to the collaborative effect of metallic Ni<sup>0</sup> centers and acidic sites within Ni<sub>3</sub>P species. Among these, metallic Ni<sup>0</sup> sites activated formic acid and aqueous-phase glycerol to generate active hydrogen (denoted as H*); subsequently, lignin was dominantly converted into phenol and alkyl guaiacol under the comprehensive function of H*, Lewis (Ni<sup>δ+</sup> species), and Bronsted acid sites (P–OH groups). Additionally, a potential reaction pathway for CDL with 4NiP/BTD as the catalyst was suggested. This study established a feasible approach for the efficient conversion of lignin using crude glycerol and green clay resources.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"39 21","pages":"9845–9859 9845–9859"},"PeriodicalIF":5.2,"publicationDate":"2025-05-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144165846","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 & FuelsPub Date : 2025-05-16DOI: 10.1021/acs.energyfuels.5c0089510.1021/acs.energyfuels.5c00895
Arooj Nisar, Arslan Hameed, Ghulam Mustafa, Guobao Xu* and Muhammad Arif Nadeem*,
{"title":"Engineered Interfaces of Nickel–Iron Nitride and Cobalt Oxide on Nitrogen-Doped Carbon Nanoribbons: A Catalytic High-Efficiency Zone for Water Splitting","authors":"Arooj Nisar, Arslan Hameed, Ghulam Mustafa, Guobao Xu* and Muhammad Arif Nadeem*, ","doi":"10.1021/acs.energyfuels.5c0089510.1021/acs.energyfuels.5c00895","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.5c00895https://doi.org/10.1021/acs.energyfuels.5c00895","url":null,"abstract":"<p >Electrocatalytic energy conversions are vital for advancing clean energy technologies, enabling processes such as water electrolysis that rely on electrochemical redox reactions at catalyst surfaces. Transition metal nitrides (TMNs) are considered as promising electrode materials due to their abundance, low cost, and noble metal-like electronic structure. In this work, we have synthesized nickel iron nitride supported over nitrogen-doped carbon nanoribbons designated as NiFeN@CoOx/N-CNRs via a facile two-step process. This involves the hydrothermal fabrication of NiFe-LDH on ZIF-12-derived CoOx/N-CNRs, followed by nitridation. The as-obtained composite NiFeN@CoOx/N-CNRs serves as a competent bifunctional electrode, delivering a current density of 20 mA/cm<sup>2</sup> at a sufficiently low overpotential (η) of 233 mV for the oxygen evolution reaction (OER) and 75 mV for hydrogen evolution reaction (HER). Moreover, it demonstrated fast reaction kinetics, minimal resistance to charge transfer (<i>R</i><sub>ct</sub>), a large electrochemically active surface area, and outstanding stability in alkaline reaction conditions for both OER and HER. These enhancements are attributed to the formation of a heterointerface between NiFeN and CoOx/N-CNRs, which facilitates superior charge migration and exploits the unique electronic properties of bimetallic nitrides. The hierarchical structure of the LDH precursor and the incorporation of N-CNRs further enhance conductivity, contributing to improved overall performance. This study provides a significant approach for fabricating and optimizing TMNs to be used as bifunctional electrodes in industrial alkaline water electrolyzers.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"39 21","pages":"9968–9980 9968–9980"},"PeriodicalIF":5.2,"publicationDate":"2025-05-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144165851","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 & FuelsPub Date : 2025-05-16DOI: 10.1021/acs.energyfuels.5c0016510.1021/acs.energyfuels.5c00165
J.P. Tiwari*,
{"title":"Outlook and Future Directions for Indoor Photovoltaics: Modern Societal Needs and Challenges","authors":"J.P. Tiwari*, ","doi":"10.1021/acs.energyfuels.5c0016510.1021/acs.energyfuels.5c00165","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.5c00165https://doi.org/10.1021/acs.energyfuels.5c00165","url":null,"abstract":"<p >The merging of research’s physical, chemical, and biological spheres is changing our way of life and human interactions. Further, artificial intelligence and the Internet of Things (IoTs) are changing our business and life interactions. This has crowded our room with several small-scale devices for daily use. The charging of all IoT devices depends on batteries. Nonetheless, self-powered IoT devices are the need of the hour. Emerging photovoltaics, known as tandem solar cells (TSCs) of silicon-perovskite, organic solar cells (OSCs), perovskite solar cells (PSCs), and silicon-perovskite combination solar cells, can provide a better solution for self-powered IoT devices. However, PSCs are coming to the forefront of this race to provide solutions for powering IoT devices. Nevertheless, every technology has its pros and cons and is in the stage of further exploration. Herein, a state-of-the-art overview of IoT-powering technology will be reviewed with a special focus on photovoltaics as the most relevant IoT-powering technology. The issues of stability and standards for emerging photovoltaic technologies are also discussed in detail for their futuristic exploration.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"39 21","pages":"9623–9640 9623–9640"},"PeriodicalIF":5.2,"publicationDate":"2025-05-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144166058","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 & FuelsPub Date : 2025-05-15DOI: 10.1021/acs.energyfuels.5c0139010.1021/acs.energyfuels.5c01390
Shanker Krishna, María Dolores Robustillo, Yu-Hao Bu, Guang-Jin Chen, Atousa Heydari, Chang-Yu Sun, Isaac Wilson and Jyoti Shanker Pandey*,
{"title":"Advancements in Key Imaging Techniques for Gas Hydrate Research to Accelerate Decarbonization Efforts","authors":"Shanker Krishna, María Dolores Robustillo, Yu-Hao Bu, Guang-Jin Chen, Atousa Heydari, Chang-Yu Sun, Isaac Wilson and Jyoti Shanker Pandey*, ","doi":"10.1021/acs.energyfuels.5c0139010.1021/acs.energyfuels.5c01390","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.5c01390https://doi.org/10.1021/acs.energyfuels.5c01390","url":null,"abstract":"<p >Gas hydrates (GHs), crystalline compounds formed by gas molecules encased in water lattices, are increasingly recognized for their dual role as both a potential energy resource and a factor in climate change, making their study pivotal to advancing decarbonization efforts. This review highlights recent advancements in imaging technologies that have significantly enhanced our understanding of GH formation, dissociation, and stability, with a focus on their implications for accelerating decarbonization. Cutting-edge techniques such as X-ray computed tomography (XCT), magnetic resonance imaging (MRI), and scanning electron microscopy (SEM) are explored for their ability to provide high-resolution structural and compositional insights. Particular emphasis is placed on microfluidics technology, which has transformed the study of GHs by enabling real-time visualization of hydrate dynamics at the pore scale under controlled conditions. The integration of micromodels with optical imaging techniques to simulate natural geological environments and investigate gas–water–hydrate interactions is discussed, alongside the impact of variables like temperature, pressure, and salinity on hydrate behavior. Furthermore, the development of in situ and real-time monitoring systems is examined for their potential to unravel the dynamic processes governing GH systems. By consolidating these advancements and addressing existing challenges, this review underscores the critical role of innovative imaging methodologies in driving research that supports decarbonization strategies through improved understanding of GH systems.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"39 21","pages":"9668–9725 9668–9725"},"PeriodicalIF":5.2,"publicationDate":"2025-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144166056","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 & FuelsPub Date : 2025-05-15DOI: 10.1021/acs.energyfuels.5c0129710.1021/acs.energyfuels.5c01297
Mingze Zhao, Bin Yuan*, Wei Zhang*, Shuhong Wu and Tianyi Fan,
{"title":"A Surrogate Model for Predicting Dynamic Reservoir Pressure Profiles in Complex Hydraulic Fracture Systems","authors":"Mingze Zhao, Bin Yuan*, Wei Zhang*, Shuhong Wu and Tianyi Fan, ","doi":"10.1021/acs.energyfuels.5c0129710.1021/acs.energyfuels.5c01297","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.5c01297https://doi.org/10.1021/acs.energyfuels.5c01297","url":null,"abstract":"<p >Dynamic intelligent prediction of the production pressure field in unconventional reservoirs aids in optimizing hydraulic fracturing designs and improving decision-making. However, traditional numerical simulation methods struggle to balance accuracy and efficiency, while most current deep-learning-based surrogate models either consider limited factors or oversimplify fracture geometries. To address these challenges, this study proposes a novel dynamic surrogate model (Dy-Pre-Net) for predicting pressure field variations during postfracturing production. The model incorporates complex hydraulic fracture geometries along with spatial data such as permeability, porosity, and the initial pressure field. It combines a channel attention mechanism with a U-Net framework to predict pressure changes across the reservoir grid. During model development, three data sets were used, and transfer learning was applied to enhance training efficiency and performance. Case studies indicate that transfer learning significantly accelerates model training. Compared with numerical simulation results, the surrogate model exhibits relatively higher absolute errors in the fracture zones and near the reservoir boundaries during the early production phase, with a maximum absolute error of up to 1.2 MPa. However, these errors gradually decrease over time. Furthermore, the surrogate model requires less than 10 s for prediction. Compared to traditional reservoir simulators, the surrogate model achieves comparable accuracy in predicting reservoir pressure fields while significantly reducing computational time.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"39 21","pages":"9828–9844 9828–9844"},"PeriodicalIF":5.2,"publicationDate":"2025-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144165953","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 & FuelsPub Date : 2025-05-15DOI: 10.1021/acs.energyfuels.5c0079210.1021/acs.energyfuels.5c00792
Beyza Yılmaz, Halide Beyza Ceylan, Gizem Yaz and Ramazan Yıldırım*,
{"title":"Performance Assessment of Catalyst Materials for CO2 Hydrogenation to Methanol Using Explainable Machine Learning","authors":"Beyza Yılmaz, Halide Beyza Ceylan, Gizem Yaz and Ramazan Yıldırım*, ","doi":"10.1021/acs.energyfuels.5c0079210.1021/acs.energyfuels.5c00792","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.5c00792https://doi.org/10.1021/acs.energyfuels.5c00792","url":null,"abstract":"<p >An extensive dataset containing 1547 data points from 84 published papers was constructed and analyzed using machine learning tools to assess the performance of catalyst materials (active metal and support). Random forest (RF) models were developed for the prediction of CO<sub>2</sub> conversion and methanol selectivity; the SHAP (SHapley Additive exPlanations) analysis, accompanying the RF models, was used to determine the contributions of descriptors, including the catalyst materials, to the conversion and selectivity predictions. Association rule mining analysis (ARM) was also utilized to determine the effects of individual catalyst material and active metal–support combinations on methanol selectivity and to improve the explainability of the results further. RF models for both CO<sub>2</sub> conversion and methanol selectivity were quite successful; the RMSE of training and testing were 2.81 (<i>R</i><sup>2</sup> = 0.87) and 3.74 (<i>R</i><sup>2</sup> = 0.74), respectively, for CO<sub>2</sub> conversion, and they were 7.31 (<i>R</i><sup>2</sup> = 0.94) and 12.74 (<i>R</i><sup>2</sup> = 0.80) for methanol selectivity. SHAP analysis indicated that the reaction temperature, the support type, the active metal type, and the catalyst preparation methods are the most significant descriptors for both CO<sub>2</sub> conversion and methanol selectivity; the temperature affects the conversion positively, while its effect on methanol selectivity is negative. ARM analysis for the catalyst material and preparation methods revealed that the use of Ga<sub>3</sub>Ni<sub>5</sub>, Ga, Ir, Ru, and Y improves methanol selectivity, while Nb<sub>2</sub>O<sub>5</sub>, CuBr<sub>2</sub>, In<sub>2</sub>O<sub>3</sub>–ZrO<sub>2</sub>, and ZnO–ZrO<sub>2</sub> are the best performing supports. The use of evaporation-induced self-assembly method and precipitation was found to be better to improve methanol selectivity. The ARM results also indicate that Cu–Nb<sub>2</sub>O<sub>5</sub>, Ga–ZnO–ZrO<sub>2</sub>, Ru–In<sub>2</sub>O<sub>3</sub>, and Y–ZrO<sub>2</sub> pairs promote high selectivity, while preparing Cu-based catalysts by precipitation and Ru-based catalyst with deposition-precipitation methods appears to be beneficial. The use of bimetallic Cu-InO<sub>2</sub>, Y–In<sub>2</sub>O<sub>3</sub>, La–In<sub>2</sub>O<sub>3</sub>, and Zn–ZrO<sub>2</sub> catalysts seems to be also beneficial.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"39 21","pages":"9956–9967 9956–9967"},"PeriodicalIF":5.2,"publicationDate":"2025-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.energyfuels.5c00792","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144165956","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}