Energy & Fuels最新文献

{"title":"Thermal Conductivity Characteristics of Porous Media in Marine Natural Gas Hydrate Reservoirs","authors":"Minghang Mao,&nbsp;Kefeng Yan*,&nbsp;Chang Chen,&nbsp;Xiaosen Li*,&nbsp;Zhaoyang Chen,&nbsp;Gang Li and Yi Wang,&nbsp;","doi":"10.1021/acs.energyfuels.4c0641810.1021/acs.energyfuels.4c06418","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.4c06418https://doi.org/10.1021/acs.energyfuels.4c06418","url":null,"abstract":"<p >As a new type of clean energy, the exploitation of natural gas hydrate resources is key in global energy development of the future. A fundamental understanding of the heat transfer characteristics of natural gas hydrate reservoirs is critical for effective natural gas hydrate exploitation. In this work, the heat transfer characteristics of the sediments on marine natural gas hydrate reservoirs were investigated by using experiments and machine learning algorithms. The thermal conductivities of natural marine sediments from the marine natural gas hydrate reservoir and their primary porous media (quartz sand, Illite, and montmorillonite) were measured. The effects of the porous media component, the water content, the salt concentration, and the phase state change on the thermal conductivity of the reservoir were discussed. The experimental results show that the thermal conductivity of the reservoir depends not only on the inherent thermal conductivity of the porous media but also on the heat transfer mode between the components. The effective thermal conductivity of the porous media system is proportional to the water content and inversely proportional to the salt concentration in porous media. The swelling characteristics of porous media affect the heat transfer mode of the system, thus affecting the extent of change in the effective thermal conductivity with variations in the water content and salt concentration. During the phase transition process, the swelling characteristics of the porous media slow down the heat transfer process, an effect that can be mitigated by the swelling inhibition caused by salt. Additionally, the performances of six machine learning algorithms were evaluated using four evaluation indicators. Results show that the gradient boosted decision trees (GBDT) can yield good predicted values of the thermal conductivity of porous media in a marine natural gas hydrate. A feature importance analysis further reveals that the salt concentration and porous media components are the essential factors influencing the thermal conductivity of marine gas hydrate reservoirs.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"39 10","pages":"4790–4806 4790–4806"},"PeriodicalIF":5.2,"publicationDate":"2025-03-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143600298","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":"Morphology, Growth Kinetics, and Porous Structure of Surfactant-Promoted Gas Hydrates: Roles of Subcooling and Surfactant Formulation","authors":"Belkacem Samar*,&nbsp;Saphir Venet,&nbsp;Arnaud Desmedt and Daniel Broseta*,&nbsp;","doi":"10.1021/acs.energyfuels.4c0625310.1021/acs.energyfuels.4c06253","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.4c06253https://doi.org/10.1021/acs.energyfuels.4c06253","url":null,"abstract":"<p >Transmission microscopy and microRaman imaging are used to investigate the morphologies, growth process, and porous structure of methane hydrate promoted by two prototypical surfactants, sodium dodecyl sulfate (SDS) and dioctyl sulfosuccinate sodium salt (AOT). Large ranges of surfactant concentrations and subcooling are considered from 100 to 1500 ppmw and 1 to 10 K. Gas hydrates are generated on the guest/water interface as hollow crystallites. These crystallites expand into the aqueous phase from their (open) basis on the interface until they detach from it to form a slurry and ultimately a porous structure, whose pores are filled with the aqueous phase. The morphologies and growth rates of those crystallites and the structure (porosity and pore sizes) of the porous medium are characterized as a function of subcooling and surfactant formulation. Under low subcooling (≈1 K), the hydrate crystallites are hollow cylinders, whose diameters decrease with increasing surfactant concentration. Under low-to-moderate subcooling (from 2 to 4 K), the crystallites are hollow spikes or cones, growing at a rate that increases with subcooling. Under high subcooling (&gt;4 K), tiny (micronic or submicronic) crystallites are massively produced at the interface. The porosity and pore sizes of the resulting porous structure decrease with increasing subcooling, down to values in the range of 40–50% and a few microns for the highest subcooling investigated (≈10 K). Rather than altering the kinetics of hydrate formation, the surfactant prevents the aggregation of hydrate crystallites on the interface as an impermeable crust and/or at the rear of the interface, thus allowing the back-flow of water and the continuous production of hydrate crystallites. In other words, the surfactant ensures the flowability of the slurry of hydrate crystallites and its removal away from the interface. These phenomena are primarily driven by the interfacial properties of the water/gas/hydrate system.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"39 10","pages":"4880–4892 4880–4892"},"PeriodicalIF":5.2,"publicationDate":"2025-03-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143600169","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":"Facile and Scalable Synthesis of Vertically Oriented TiS2 Nanosheets for Green Energy Harvesting in Microfluidic Microbial Fuel Cells","authors":"S. Ahmad Etghani*,&nbsp;Mohammad Hosseini,&nbsp;Mir Razi Mousavi,&nbsp;Ehsan Ansari,&nbsp;Zeinab Sanaee and Shams Mohajerzadeh*,&nbsp;","doi":"10.1021/acs.energyfuels.4c0596710.1021/acs.energyfuels.4c05967","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.4c05967https://doi.org/10.1021/acs.energyfuels.4c05967","url":null,"abstract":"<p >Employing inexpensive and achievable nanomaterials in energy devices is essential due to the demands for miniaturization and high storage capacity. Addressing the challenge of large-scale synthesis and introducing new affordable materials with promising charge acquisition and retention capabilities can significantly advance energy generation technologies. Here, we introduce vertically aligned 2D nanosheets of titanium disulfide (TiS₂) as a new material for anode electrodes in microbial fuel cells (MFCs). We present a novel, scalable, and facile synthesis method that utilizes a sacrificial titanium layer in a chemical vapor deposition-based approach, facilitating the large-area vertical growth of TiS₂ nanosheets without the use of hazardous precursors. The semimetallic properties of these nanosheets, combined with their distinctive 3D configuration, enhance both bacterial colonization and electron transfer efficiency. The performance of TiS₂ nanosheets was evaluated in a microfluidic-based MFC system with <i>Escherichia coli</i> as the microorganism. Comprehensive assessments, including polarization curves and cell potential measurements, demonstrate a peak power density of 169.4 W m^–3 and a current density of 1270 A m^–3 under optimal conditions. The 3D electrode, featuring TiS₂ nanosheets, maintains robust power generation at high current densities, highlighting its effective electrode–electrolyte interaction and charge transfer facilitation.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"39 10","pages":"4834–4848 4834–4848"},"PeriodicalIF":5.2,"publicationDate":"2025-02-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143600352","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":"Nucleation Probability of Methane + Propane Mixed-Gas Hydrate Depending on Gas Composition","authors":"Tsutomu Uchida*,&nbsp;Masato Hayama,&nbsp;Motoi Oshima and Kenji Yamazaki,&nbsp;","doi":"10.1021/acs.energyfuels.4c0636910.1021/acs.energyfuels.4c06369","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.4c06369https://doi.org/10.1021/acs.energyfuels.4c06369","url":null,"abstract":"<p >Gas hydrates show promise as gas storage and transportation media. But before using them in such industries, we should learn how to better control their formation. In particular, their nucleation is stochastic and requires either high supersaturation or long induction times. Here we study experimentally how the induction time varies with the gas composition using methane (CH₄) + propane (C₃H₈) mixed-gas hydrate as a mimic of natural gas. We form CH₄ + C₃H₈ mixed-gas hydrates with a composition ratio CH₄:C₃H₈ ranging from 100:0 to 0:100 in a high-pressure vessel with a stirring system at a constant temperature of about 274.7 K. The induction time is determined as the time period from the start of stirring to the hydrate formation defined by either a sudden temperature rise or a pressure drop in the vessel. To obtain quantitative nucleation data, we repeated at least 10 experiments for each condition. Compared to that of pure CH₄ hydrate, the induction time of CH₄ + C₃H₈ mixed-gas hydrate is found to be significantly shorter when C₃H₈ is present at even 1% in the vapor. Then, we quantify the stochastic nucleation process as the composition-dependent nucleation frequency. As a result, we show that the nucleation frequency of CH₄ + C₃H₈ mixed-gas hydrate exponentially decreases with increasing C₃H₈ in vapor. This behavior correlates well with the composition dependence of the empty-cage ratio in the gas hydrate. Based on these results, we propose a model for the nucleation of mixed-gas hydrates.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"39 10","pages":"4782–4789 4782–4789"},"PeriodicalIF":5.2,"publicationDate":"2025-02-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143600360","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":"Direct Prelithiation of Silicon-Based Composite Electrodes via Island-like Thermal Evaporation","authors":"Amanda L. Musgrove*,&nbsp;Katie L. Browning,&nbsp;Robert L. Sacci,&nbsp;Andrew Ullman,&nbsp;Harry M. Meyer III,&nbsp;Kyle Musgrove,&nbsp;Joseph Quinn,&nbsp;Sören Möller,&nbsp;Martin Finsterbusch and Gabriel M. Veith*,&nbsp;","doi":"10.1021/acs.energyfuels.4c0611310.1021/acs.energyfuels.4c06113","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.4c06113https://doi.org/10.1021/acs.energyfuels.4c06113","url":null,"abstract":"<p >Irreversible losses of Li during solid electrolyte interface (SEI) conditioning in batteries are a key contributor to the lower specific capacities observed in silicon-containing Li-ion batteries. Herein, thermal evaporation of between 1 and 20 μm of Li onto Si-based composite anodes has been investigated as a prelithiation method to compensate for such losses. Additionally, to account for mechanical strain caused by Li–Si alloying and electrode expansion during the deposition, a stainless-steel mesh is applied to the electrodes before prelithiation to form “island-like” deposition on the electrode surface. The open circuit potential was also found to decrease as a function of increased Li evaporation, consistent with the potentials of electrochemically prepared Li_<i>x</i>Si alloys. Prelithiating to compensate for irreversible Li losses to SEI formation resulted in full cells with a 15.8% increase in initial Coulombic efficiency and a 47.8% reduction in irreversible capacity loss after SEI formation cycling. Subsequent C/3 cycling showed up to a 62.9% increase in the specific capacity in prelithiated cells. X-ray photoelectron spectroscopy (XPS) revealed differences in the SEI composition that was formed by electrochemical cycling and reactively formed in prelithiated cells upon exposure to the Gen2 + 3% FEC electrolyte. The reactively formed SEI from the spontaneous reaction with lithiated silicon was carbonate-rich, while the electrochemical SEI formation showed significantly more LiPF_<i>x</i> species, which could play a role in overall cycling performance.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"39 10","pages":"4968–4982 4968–4982"},"PeriodicalIF":5.2,"publicationDate":"2025-02-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143600362","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":"Enhanced Coal Bed Methane (ECBM) Recovery by Injecting Different Gas Components","authors":"Haiou Wen,&nbsp;Chaojun Fan*,&nbsp;Lijun Zhou,&nbsp;Lei Yang,&nbsp;Xiang Fu,&nbsp;Mingkun Luo,&nbsp;Huijie Shi,&nbsp;Yiqi Wang and Gang Bai,&nbsp;","doi":"10.1021/acs.energyfuels.5c0021110.1021/acs.energyfuels.5c00211","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.5c00211https://doi.org/10.1021/acs.energyfuels.5c00211","url":null,"abstract":"<p >In order to investigate the effects of different injected gas components for enhancing coalbed methane (ECBM), a multifield coupling system is independently developed for the gas injection displacement of coal-containing gas under stress loading. Experimental research has been conducted on the effects of different injection gas components, including flue gas, mixture, N₂, CO₂, and air for the ECBM experiments. The results show that according to the variation law of each gas volume fraction in the gas mixture at the outlet of the triaxial pressure chamber, ECBM can be divided into four stages. Stage I: the volume fraction of CH₄ is maintained at 100%. Stage II: N₂ breaks through the coal sample; the gas is a mixture of CH₄ and N₂ gas. Stage III: O₂ breaks through; the gas is a mixture of CH₄, N₂, and O₂ gas. Stage IV: CO₂ breaks through; the gas is a mixture of CH₄, CO₂, O₂, and N₂ gas with gradually increasing CO₂. Additionally, when N₂, air, and flue gas are injected into coal samples, the instantaneous flow shows an L-shaped pattern of “rapid decrease-slow decrease-maintain constant”. However, when coal samples are injected with a mixture and CO₂, the instantaneous gas flow shows a V-shaped pattern of “rapid decrease-slow decrease-slow increase-maintain constant”. The CH₄ recovery rate is finally of the order CO₂ &gt;mixture &gt; flue gas &gt; air&gt; N₂, with 99.6, 95.5, 93.1, 90.0, and 88.5%, respectively. Therefore, the higher the volume fraction of CO₂ in the injected gas component, the more thorough the desorption of CH₄, and the longer the time required for ECBM.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"39 10","pages":"4807–4817 4807–4817"},"PeriodicalIF":5.2,"publicationDate":"2025-02-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143600353","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":"Study on Emulsification of Heavy Oil in Porous Media","authors":"Jiajing Chang*,&nbsp;Zhaojie Song,&nbsp;Bingyu Ji,&nbsp;Zengmin Lun,&nbsp;Yongqiang Tang and Yibin Qi,&nbsp;","doi":"10.1021/acs.energyfuels.4c0503310.1021/acs.energyfuels.4c05033","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.4c05033https://doi.org/10.1021/acs.energyfuels.4c05033","url":null,"abstract":"<p >The existence of an emulsion can greatly improve the oil displacement efficiency, which has important practical significance for the development of heavy oil reservoirs. However, the description of the emulsification phenomenon is basically based on the observation of produced fluid and the monitoring of pressure points along the way. The actual emulsification in the porous media cannot be observed. In this paper, the emulsification phenomenon of heavy oil in porous media was studied by <i>D</i>–<i>T</i>₂ two-dimensional spectrum. In this study, the <i>D</i>–<i>T</i>₂ two-dimensional spectral characteristics of free water, water-in-oil (W/O) emulsions, and oil-in-water (O/W) emulsions were first studied. Second, the <i>D</i>–<i>T</i>₂ two-dimensional spectrum characteristics of emulsions at different temperatures in nonporous media were studied. Finally, the <i>D</i>–<i>T</i>₂ two-dimensional spectrum characteristics of emulsions at different temperatures in porous media were studied. The results showed that at the reservoir temperature, the oil peak and water peak on the <i>D</i>–<i>T</i>₂ two-dimensional spectrum were on both sides of the boundary of the diffusion coefficient of 8 × 10^–10 m²/s, and the diffusion coefficient of oil was much smaller than 8 × 10^–10 m²/s, while the diffusion coefficient of water was still much larger than 8 × 10^–10 m²/s even if it was affected by confined diffusion in the core. In the <i>D</i>–<i>T</i>₂ 2D spectrum, the water signal of free water fell on the free water line; the water signal of W/O emulsion fell below the free water line. The water signal of O/W emulsion was not far from the free water line. The lower the temperature, the apparent diffusion coefficient of water for W/O emulsion was smaller. On the contrary, the higher the temperature, the apparent diffusion coefficient of water for O/W emulsions was smaller. The <i>D</i>–<i>T</i>₂ two-dimensional spectrum characteristics of emulsions in porous media and nonporous media at different temperatures were similar, but the presence of porous *media further reduced the apparent diffusion coefficient of water. The results of this study can more accurately predict and guide the quality and efficiency improvement of heavy oil reservoirs.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"39 10","pages":"4728–4745 4728–4745"},"PeriodicalIF":5.2,"publicationDate":"2025-02-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143600354","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":"Review on Photocatalytic Oxidation of Hg0 by BiOIO3-Based Materials","authors":"Tongtong Guan,&nbsp;Zhou Shi,&nbsp;Bin Chen,&nbsp;Wenquan Zhou,&nbsp;Sorachon Yoriya,&nbsp;Ping He*,&nbsp;Chaoen Li*,&nbsp;Jiang Wu*,&nbsp;Yang Ling,&nbsp;Guangyang An,&nbsp;Jingxian Du and Jinghan Yang,&nbsp;","doi":"10.1021/acs.energyfuels.4c0598910.1021/acs.energyfuels.4c05989","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.4c05989https://doi.org/10.1021/acs.energyfuels.4c05989","url":null,"abstract":"<p >Photocatalytic oxidation of Hg⁰ is an environmental protection technology that removes Hg⁰ from flue gas by oxidizing Hg⁰ using active species produced by photocatalysts under light conditions. For the past few years, BiOIO₃ has drawn a lot of attention from scientists because of its special layered structure and internal polarity. In this work, we first introduce the photoelectrochemical properties of BiOIO₃, and the modification methods of BiOIO₃ are summarized according to different photocatalytic mercury oxidation mechanisms. Second, density functional theory is used to calculate the energy bands, density of states, and work function to reveal the changes in the microscopic physicochemical properties of the modified catalysts. Then, the synthesis methods of BiOIO₃ and its composites are summarized and the effects of different flue gas components on the photocatalytic oxidation of Hg⁰ are investigated. Finally, the applications of BiOIO₃ in other fields are briefly introduced, suggesting that the use of such catalysts for synergistic treatment in the fields of mercury removal and carbon dioxide reduction is a direction to be explored in the future. Furthermore, the modification of the BiOIO₃ series catalysts according to their unique layered structure will be the next focus of their use in photocatalytic mercury oxidation. This work contributes to the development of more efficient BiOIO₃ series photocatalysts.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"39 10","pages":"4648–4668 4648–4668"},"PeriodicalIF":5.2,"publicationDate":"2025-02-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143600361","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":"Advances and Perspectives in ZIF-67 Synthesis for Hydrogen Applications: A Review","authors":"Aaush Bhardwaj Singh,&nbsp; and ,&nbsp;Manishkumar D. Yadav*,&nbsp;","doi":"10.1021/acs.energyfuels.4c0586710.1021/acs.energyfuels.4c05867","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.4c05867https://doi.org/10.1021/acs.energyfuels.4c05867","url":null,"abstract":"<p >Metal–organic frameworks (MOFs), notably Zeolitic Imidazolate Framework-67 (ZIF-67) and its derivatives, have garnered significant attention as versatile materials due to their distinct structural properties, including high surface area, open crystal structure, and tunable pore structures. ZIF-67 has been synthesized through various methods and intensification techniques, contributing to a vast amount of literature on their synthesis. This Review presents a thorough examination of synthesis methods, incorporating recent advancements, and explores the factors influencing the morphological and structural characteristics of ZIF-67. The paper outlines various intensification techniques for the synthesis of ZIF-67. Moreover, it addresses the challenges associated with the industrial-scale production of such materials and discusses the importance of reproducibility studies in ensuring consistency and reliability. Furthermore, the paper delves into the engineering aspects of ZIF-67 production and elaborates on the potential of ZIF-67 in the critical domain of hydrogen storage. This Review aims to offer comprehensive insight into the current state-of-the-art in ZIF-67 research, encouraging further exploration and innovation in this dynamic field.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"39 10","pages":"4610–4647 4610–4647"},"PeriodicalIF":5.2,"publicationDate":"2025-02-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143600247","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 New Doped Graphene-Based Catalyst for Hydrogen Evolution Reaction Under Low-Electrolyte Concentration and Biomass-Rich Environments","authors":"I. Vidal-Barreiro*,&nbsp;P. Sánchez*,&nbsp;A. de Lucas-Consuegra* and A. Romero*,&nbsp;","doi":"10.1021/acs.energyfuels.4c0608410.1021/acs.energyfuels.4c06084","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.4c06084https://doi.org/10.1021/acs.energyfuels.4c06084","url":null,"abstract":"<p >Graphene-based catalysts are emerging as promising alternatives to reduce reliance on metal-based catalysts in the hydrogen evolution reaction (HER). This study introduces a novel family of metal-free graphene-based materials codoped with nitrogen and phosphorus (GNP). These materials were synthesized, characterized, and evaluated for HER performance as glucose-tolerant cathodes for biomass electrolysis in a soft alkaline medium, referred to as Mixed Electrolyte (ME): 0.1 M NaOH + 1.0 M Na₂SO₄. It was found that the calcination time directly affects the catalytic properties of the final catalysts, with longer calcination times enhancing HER activity. This was attributed to the effective incorporation of nitrogen (N pyrrolic, N quaternary) and phosphorus (P graphitic) into the graphitic network, along with increased catalyst mesoporosity, which significantly improves mass and electron transfer. Furthermore, chronopotentiometry tests revealed substantial electrochemical activation of HER catalytic performance, stemming from the removal of heteroatoms from the carbon framework. This process, confirmed by XPS and Raman Spectroscopy, led to the formation of topological 5- and 7-membered carbon rings, which serve as the main active sites for the reaction. This significantly accelerates the water dissociation activity, leading to improved catalytic performance with a final overpotential (η₁₀) of −0.386 V in ME. Notably, the exceptional stability and electrochemical activity under various alkaline media, along with its tolerance in the presence of glucose, make this new cathodic catalyst a suitable candidate for a membrane-less biomass electrolyzer.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"39 9","pages":"4515–4524 4515–4524"},"PeriodicalIF":5.2,"publicationDate":"2025-02-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143547693","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}