Energy & FuelsPub Date : 2025-03-18DOI: 10.1021/acs.energyfuels.4c0486910.1021/acs.energyfuels.4c04869
Elvin Mirzayev, Mustafa Al Ramadan*, Murtada Saleh Aljawad*, Ahmed Farid Ibrahim, Zuhair Al-Yousif and Ahmed Al Yaseri,
{"title":"A Study of the Optimum Injection Rate of CO2-Saturated Brine in Limestone Aquifers and Its Impact on Rock Geomechanics","authors":"Elvin Mirzayev, Mustafa Al Ramadan*, Murtada Saleh Aljawad*, Ahmed Farid Ibrahim, Zuhair Al-Yousif and Ahmed Al Yaseri, ","doi":"10.1021/acs.energyfuels.4c0486910.1021/acs.energyfuels.4c04869","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.4c04869https://doi.org/10.1021/acs.energyfuels.4c04869","url":null,"abstract":"<p >Deep saline aquifers are promising locations for carbon sequestration, but the impact of the CO<sub>2</sub> injection rate on rock properties requires careful investigation. This study examines the effects of CO<sub>2</sub>-saturated brine injection on limestone, specifically analyzing how the injection rate influences wormhole formation and subsequent changes in petrophysical and geomechanical properties. Various injection rates were employed to investigate the impact of the injection rate, ranging from 0.25 to 5 cm<sup>3</sup>/min, for the coreflooding experiments. Before and after coreflooding, the Young’s modulus (YM) and Poisson’s ratio of the samples were measured at various confining pressures. Additionally, the porosity and the permeability of the treated samples were assessed. A micro-CT scan was employed to visualize the generated wormholes and quantify their volumes to calculate the Damkohler number. Our study revealed that among the five tested injection rates 1 cm<sup>3</sup>/min resulted in the lowest pore volumes to breakthrough (PVBT). We employed the Buijse and Glasbergen model, curve-fitting our data to determine the optimum velocity for CO<sub>2</sub>-saturated brine, which was found to be 0.4 cm/min (equivalent to an injection rate of 0.75 cm<sup>3</sup>/min). All samples showed a noticeable change in rock YM, with the rock exposed to a 5 cm<sup>3</sup>/min injection rate showing the least reduction. Furthermore, our experiments revealed that conventional methods for determining the optimum conditions for wormhole formation, such as the Buijse and Glasbergen model and the generalized curve using the Damkohler number, are insufficient for accurately predicting wormhole formation in CO<sub>2</sub>-saturated brine. The experiments demonstrated a significant deviation from the expected behavior in terms of the generalized curve. Additionally, the Buijse and Glasbergen model overestimated PVBT at interstitial velocities lower than the predicted optimum. These findings underscore the need for alternative approaches to accurately predict wormholing phenomena, specifically in CO<sub>2</sub> storage applications, where the brine is saturated with CO<sub>2</sub>.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"39 12","pages":"5754–5766 5754–5766"},"PeriodicalIF":5.2,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143703706","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 : 2025-03-18DOI: 10.1021/acs.energyfuels.4c0510610.1021/acs.energyfuels.4c05106
Yakov Shitrit, Tomer Karmel, Sonal Rajput, Yaron S. Cohen and Eran Edri*,
{"title":"Catalytic Layer Microstructure in Pulsed Electrodeposited Bismuth-Based Gas Diffusion Electrodes Used for CO2 Reduction to Formate","authors":"Yakov Shitrit, Tomer Karmel, Sonal Rajput, Yaron S. Cohen and Eran Edri*, ","doi":"10.1021/acs.energyfuels.4c0510610.1021/acs.energyfuels.4c05106","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.4c05106https://doi.org/10.1021/acs.energyfuels.4c05106","url":null,"abstract":"<p >The electrochemical carbon dioxide reduction (CO<sup><sub>2</sub></sup>r) reaction offers a viable method for converting waste carbon dioxide into valuable products. Gas diffusion electrodes (GDEs) are crucial for meeting the high current density demands associated with the upscaling of CO<sub>2</sub>r. In this research, we investigated how the microstructure of the catalytic layer in a Bi-based GDE and the catalyst nanostructure can be modified by altering the electrodeposition duty cycle. Furthermore, we explored how the microstructure influences the key performance indicators of the GDE. The outcomes demonstrated that decreasing the duty cycle of pulsed electrodeposition enhances the catalyst dispersibility within the three-dimensional catalytic layer, thereby improving catalytic performance. Additionally, reducing the duty cycle increased the nucleation site density, leading to smaller catalysts and denser catalytic sites, further enhancing the catalytic performance. By employing a Sustainion ionomer and a 60–80 μm thick catalytic layer, we achieved a current density exceeding −210 mA/cm<sup>2</sup> (at −1.0 V vs RHE) with 100% Faradaic efficiency for formate in a semi-batch testing bed. This research provides novel insights into catalytic layer design and offers a strategy to modify it to meet the stringent industrial benchmarks.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"39 12","pages":"5965–5973 5965–5973"},"PeriodicalIF":5.2,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.energyfuels.4c05106","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143703702","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 : 2025-03-18DOI: 10.1021/acs.energyfuels.4c0589010.1021/acs.energyfuels.4c05890
Xuechi Liu, Pengfei Wang, Zhouhua Wang, Shouheng Xiao, Meng Han, Bao Yuan*, Songbai Han, Jinlong Zhu* and Yun Li*,
{"title":"Methane Hydrate Formation in the Confined Nanochannel of Graphene-Mica Slits: Insights from Molecular Dynamics Simulation Study","authors":"Xuechi Liu, Pengfei Wang, Zhouhua Wang, Shouheng Xiao, Meng Han, Bao Yuan*, Songbai Han, Jinlong Zhu* and Yun Li*, ","doi":"10.1021/acs.energyfuels.4c0589010.1021/acs.energyfuels.4c05890","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.4c05890https://doi.org/10.1021/acs.energyfuels.4c05890","url":null,"abstract":"<p >The impact of hydrophilic and hydrophobic surfaces and their confined space on the nucleation and growth of gas hydrates is an important topic in hydrate formation research. This study employed molecular dynamics simulations to investigate the nucleation and growth mechanisms of methane hydrate (MH) within the confined space between graphene and mica. The results demonstrate that MH formation is influenced by the methane mole fraction and the pore size of the graphene-mica nanochannel. Higher methane mole fractions led to an increased number of MH cages. Methane molecules were adsorbed onto the graphene surface, while the water molecules accumulated on the mica surface due to the hydration properties of K<sup>+</sup> cations. Furthermore, methane cannot penetrate the hydrated structures of K<sup>+</sup> on the mica surface, leading to the formation of stable MH cages in the central region of the graphene-mica nanochannel. This study reveals the nucleation and growth mechanisms of MH within the confined space formed by graphene and the mica surface. These findings are significant for advancing the understanding and control of gas hydrate formation on hydrophilic and hydrophobic surfaces.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"39 12","pages":"5707–5718 5707–5718"},"PeriodicalIF":5.2,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143703692","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 : 2025-03-18DOI: 10.1021/acs.energyfuels.4c0596510.1021/acs.energyfuels.4c05965
Nitish Srivastava, Mohammad Saquib, Pratham Arora and Amit C. Bhosale*,
{"title":"Investigation of NiMoSe/Ti3C2Tx on Carbon Cloth as an Effective Electrocatalyst for the Hydrogen Evolution Reaction in an Acidic Medium","authors":"Nitish Srivastava, Mohammad Saquib, Pratham Arora and Amit C. Bhosale*, ","doi":"10.1021/acs.energyfuels.4c0596510.1021/acs.energyfuels.4c05965","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.4c05965https://doi.org/10.1021/acs.energyfuels.4c05965","url":null,"abstract":"<p >Hydrogen has the potential to play a pivotal role in decarbonizing the energy sector. Electrochemical water splitting encompasses the hydrogen evolution reaction (HER) at the cathode utilizing platinum as a catalyst owing to its extraordinary performance. Nevertheless, low-cost, efficient, and stable electrocatalysts are required due to the high cost and scarcity of platinum. In the present study, a hydrothermally synthesized NiMoSe/Ti<sub>3</sub>C<sub>2</sub>T<sub><i>x</i></sub> composite grown on activated carbon cloth (CC) has been investigated for its efficacy toward HER in an acidic medium (0.5 M H<sub>2</sub>SO<sub>4</sub>). Techniques such as X-ray diffraction, X-ray photoelectron spectroscopy, scanning electron microscopy, and transmission electron microscopy have been incorporated to confirm and characterize the synthesis on CC. Consequently, the atomic ratio of Ni/Mo/Se/Ti has been determined as 1:2.78:3.12:1.06. Electrochemical characterization reveals an overpotential of 403 mV at −10 mA (η<sub>10</sub>) as compared to 202 mV for commercial Pt/C (40%) and a Tafel slope of 33 mV dec<sup>–1</sup> as opposed to 28 mV dec<sup>–1</sup> for Pt/C. The use of MXene has a positive effect on the stability of the composite (49 mV increase in overpotential after 1000 cycles). Furthermore, a detailed economic and cradle-to-gate life cycle assessment has been done for the synthesized electrocatalyst, revealing a cost saving of 88.4% and a global warming potential of 0.15148 kg CO<sub>2</sub>/(mg cm<sup>–2</sup>). The synthesized electrocatalyst can thus be used as a cost-effective and efficient catalyst for electrochemical water splitting at the cathode.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"39 12","pages":"5719–5729 5719–5729"},"PeriodicalIF":5.2,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143703705","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 : 2025-03-18DOI: 10.1021/acs.energyfuels.5c0020910.1021/acs.energyfuels.5c00209
Yifan Li, and , Jun Yao*,
{"title":"Phase Transition Mechanisms of Hydrocarbons in Nanopores of Shale Formation","authors":"Yifan Li, and , Jun Yao*, ","doi":"10.1021/acs.energyfuels.5c0020910.1021/acs.energyfuels.5c00209","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.5c00209https://doi.org/10.1021/acs.energyfuels.5c00209","url":null,"abstract":"<p >To gain a deep understanding of the phase transition mechanisms of confined hydrocarbons, we first use the molecular dynamics simulations to model the phase transition process of hydrocarbons induced by temperature changes. The results show that the phase transition rates of confined hydrocarbons vary at different locations due to heterogeneous strength exerted by pore walls, which enables pure hydrocarbons to exhibit a multiphase coexistence state within the nanopores. Then, Grand Canonical Monte Carlo simulations were preformed to study the pore size effect and interfacial effect of <i>n</i>-pentane in nanopores. The pore size effect primarily influences the volume fraction of the adsorbed phase, while the interfacial effect regulates the density of the adsorption layers. This research provides theoretical insights into the phase behavior characteristic and phase transition mechanism of hydrocarbons in nanopores, which is significant for improving the recovery of shale oil and gas resources.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"39 12","pages":"5730–5740 5730–5740"},"PeriodicalIF":5.2,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143703701","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 : 2025-03-18DOI: 10.1021/acs.energyfuels.4c0582810.1021/acs.energyfuels.4c05828
Wallace P. Morais, Guilherme J. Inacio, Eduardo A. R. de Almeida, Fábio A. L. de Souza, Fernando N. N. Pansini and Wendel S. Paz*,
{"title":"CO2 Reduction Reactivity on the SiC Monolayer with Doped Topological Defects","authors":"Wallace P. Morais, Guilherme J. Inacio, Eduardo A. R. de Almeida, Fábio A. L. de Souza, Fernando N. N. Pansini and Wendel S. Paz*, ","doi":"10.1021/acs.energyfuels.4c0582810.1021/acs.energyfuels.4c05828","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.4c05828https://doi.org/10.1021/acs.energyfuels.4c05828","url":null,"abstract":"<p >This study explores the catalytic properties of boron- and nitrogen-doped 585 extended line defects (585-ELD) in SiC monolayers for the CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR). Using Density Functional Theory and <i>ab initio</i> Molecular Dynamics (AIMD) simulations, we analyze the stability, electronic structure, and adsorption characteristics of each doped defect. The results indicate that all doped systems, except for N–N, exhibit significant kinetic and thermodynamic stability, with midgap states that enhance electron availability and catalytic activity. Among the doped structures, the C–B ELD system uniquely balances CO<sub>2</sub> protonation and H<sub>2</sub> desorption, selectively favoring CO<sub>2</sub> reduction over hydrogen evolution. Calculated reaction free energies show that CH<sub>4</sub> formation is possible if the transition from H<sub>2</sub>COH to CH<sub>2</sub> occurs, with a limiting potential (<i>U</i><sub><i>L</i></sub>) of 0.73 V, while strong interactions between H<sub>2</sub>COH and the surface make CH<sub>3</sub>OH formation energetically challenging. These findings position the C–B ELD SiC system as a promising candidate for efficient and selective CO<sub>2</sub> conversion, enabling the formation of valuable hydrocarbons and oxygenates through effective charge transfer and controlled reaction pathways.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"39 12","pages":"5767–5777 5767–5777"},"PeriodicalIF":5.2,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.energyfuels.4c05828","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143703720","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}
{"title":"Quantifying the Limits of CH4–CO2 Hydrate Replacement: Impact of Critical Replacement Thickness, Particle Size, and Flow Rate on Recovery Efficiency","authors":"Jin-Rong Zhong, Kai-Bo Huang, Shan Yang, Zuo-Zhi Luo, Ya-Xuan Zhu, Li Wan, Yi-Fei Sun, Chang-Yu Sun, Guang-Jin Chen and Yue-Fei Zhang*, ","doi":"10.1021/acs.energyfuels.5c0037110.1021/acs.energyfuels.5c00371","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.5c00371https://doi.org/10.1021/acs.energyfuels.5c00371","url":null,"abstract":"<p >The CH<sub>4</sub>–CO<sub>2</sub> hydrate replacement exploitation method has gained high attention, but its low recovery efficiency hampers its application, and the reported limits of CH<sub>4</sub>–CO<sub>2</sub> replacement vary greatly among different studies. This study introduces the concept of critical replacement thickness to quantify the exploitation limits of CH<sub>4</sub>–CO<sub>2</sub> hydrate replacement, based on a series of CH<sub>4</sub>–CO<sub>2</sub> replacement experiments conducted in a one-dimensional high-pressure reactor with well-defined hydrate-bearing sediments. Real-time hydrate composition analysis was employed to calculate the CH<sub>4</sub>–CO<sub>2</sub> replacement limitation and critical replacement thickness at various stages of CO<sub>2</sub> flooding. The results show that during the initial stage, the replacement thickness is approximately 2–4 μm, while it decreases to 0.1–0.3 μm in the final stage. Additionally, the study systematically examines the impact of the hydrate particle size and fluid flow rate on CH<sub>4</sub> recovery and CO<sub>2</sub> sequestration. It is found that smaller particle sizes and higher flow rates significantly improve recovery efficiency, with CH<sub>4</sub> recovery increasing from 39.1 to 63.4% through optimization of these factors. Moreover, the mass transfer resistance created by the reformed CH<sub>4</sub>–CO<sub>2</sub> hydrate film restricts the critical replacement thickness to no more than 7 μm for a particle size distribution of 0–250 μm without additional stimulation. The findings provide a clearer understanding of the factors influencing CH<sub>4</sub> recovery and offer insights into optimizing the replacement method for improved efficiency. These results contribute to the development of more effective strategies for the CH<sub>4</sub>–CO<sub>2</sub> replacement exploitation in hydrate reservoirs.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"39 12","pages":"5741–5753 5741–5753"},"PeriodicalIF":5.2,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143703750","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 : 2025-03-17DOI: 10.1021/acs.energyfuels.4c0578310.1021/acs.energyfuels.4c05783
Shuxin Li, Qiyuan Yang and Kareem Bachagha*,
{"title":"High-Performance Polymer Solar Cells Based on Blue-Light-Emitting Polyfluorene Derivative-Doped Systems","authors":"Shuxin Li, Qiyuan Yang and Kareem Bachagha*, ","doi":"10.1021/acs.energyfuels.4c0578310.1021/acs.energyfuels.4c05783","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.4c05783https://doi.org/10.1021/acs.energyfuels.4c05783","url":null,"abstract":"<p >The polymer solar cells (PSCs) have received a lot of research attention owing to their commendable qualities. However, the insufficient photoelectric conversion efficiency restricts their application and popularization, among which the existing problems can be summarized as low optical absorption leading to low spectral utilization of the device and the charge transfer obstructed due to energy level mismatch. Therefore, broadening the light absorption range of the active layer and promoting carrier transmission are the keys to improving the device performance. We synthesized blue polyfluorene derivatives containing a phenoxazine unit (PF-PO) and introduced in a PSC system based on PM6:IT-4F blends to improve the absorbance and improve the exciton dissociation efficiency and balanced charge carrier mobility. The power conversion efficiency (PCE) of the device improved from 12.64% when undoped to 13.97% after doping with PF-PO. The short-circuit density (<i>J</i><sub>SC</sub>) is improved from 21.23 to 22.47 mA/cm<sup>2</sup>, and the fill factor (FF) is improved from 70.31 to 73.16%, which is the main factor for the improvement of device efficiency. These findings suggest that incorporating doping into the device is a highly effective method for improving the photovoltaic performance of the material.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"39 12","pages":"5947–5955 5947–5955"},"PeriodicalIF":5.2,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143703785","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 : 2025-03-17DOI: 10.1021/acs.energyfuels.4c0600210.1021/acs.energyfuels.4c06002
Zihao Feng, Ruixin He, Qiang Zhang, Xiuzhi Han, Yang Yue, Guangren Qian and Jia Zhang*,
{"title":"Enhanced SO2-Resistance Ability of Ce-Modified TiO2-Wrapped V2O5 Catalyst","authors":"Zihao Feng, Ruixin He, Qiang Zhang, Xiuzhi Han, Yang Yue, Guangren Qian and Jia Zhang*, ","doi":"10.1021/acs.energyfuels.4c0600210.1021/acs.energyfuels.4c06002","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.4c06002https://doi.org/10.1021/acs.energyfuels.4c06002","url":null,"abstract":"<p >SO<sub>2</sub>-resistance ability is critical for a catalyst since SO<sub>2</sub> usually coexists in polluted gas and results in catalyst deactivation. In this work, structural design and Ce modification methods are utilized to synthesize a Ce-modified TiO<sub>2</sub>-wrapped V<sub>2</sub>O<sub>5</sub> catalyst, and its performance is verified in the selective catalytic reduction of nitrogen oxide (SCR). As a result, the wrapped structure (Ti/V<sub>S</sub>) and Ce modification (CeTi/V<sub>S</sub>) not only increase the conversion but also enhance the SO<sub>2</sub>-resistance ability. Under the same V amount and catalysis conditions, Ti/V<sub>S</sub> reaches a removal rate of 60% at 250 °C, which is higher than that (55%) of the typical V-supported TiO<sub>2</sub> (V/Ti). The conversion of CeTi/V<sub>S</sub> is further increased to 72%. After SO<sub>2</sub> deactivation, conversions follow the order of 25% (V/Ti) < 38% (Ti/V<sub>S</sub>) < 52% (CeTi/V<sub>S</sub>). In addition, SO<sub>2</sub> deactivation is easier to reduce in the two wrapped catalysts under thermal regeneration. After detailed characterizations of surface elements and SCR intermediates, the mechanism for the enhanced SO<sub>2</sub>-resistance ability is revealed. In brief, SO<sub>2</sub>-derived species on Ti/V<sub>S</sub> are replaceable by nitrogen oxide, and Ce-combined SO<sub>2</sub> in CeTi/V<sub>S</sub> functions as new sites for SCR. Besides, the two wrapped catalysts have larger specific surface areas than V/Ti. The main result of this work is devoted to understanding the structure–function relationship, which is also in favor of promoting catalyst application.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"39 12","pages":"5886–5896 5886–5896"},"PeriodicalIF":5.2,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143703784","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 : 2025-03-17DOI: 10.1021/acs.energyfuels.4c0641210.1021/acs.energyfuels.4c06412
Jiawang Liu, Yi Zeng, Yuemiao Lai, Xiao Chen, Tao Wang*, Fangliang Li* and Qing Guo*,
{"title":"Low-Temperature Photooxidation of Ethylene on Rutile TiO2(110)","authors":"Jiawang Liu, Yi Zeng, Yuemiao Lai, Xiao Chen, Tao Wang*, Fangliang Li* and Qing Guo*, ","doi":"10.1021/acs.energyfuels.4c0641210.1021/acs.energyfuels.4c06412","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.4c06412https://doi.org/10.1021/acs.energyfuels.4c06412","url":null,"abstract":"<p >The conversion of ethylene (C<sub>2</sub>H<sub>4</sub>) with photocatalysis provides an alternative to traditional C<sub>2</sub>H<sub>4</sub> conversion into acetaldehyde (CH<sub>3</sub>CHO) processes in industrial production. Herein, low-temperature C<sub>2</sub>H<sub>4</sub> oxidation is conducted on rutile (R)-TiO<sub>2</sub>(110) under the third-harmonic (343 nm) and fourth-harmonic (257 nm) outputs of the laser. The results illustrate that both hole-trapped bridging oxygen (O<sub>b</sub><sup>–</sup>) and Ti<sub>5c</sub> bound oxygen adatom (O<sub>Ti</sub><sup>–</sup>) are photoactive for C<sub>2</sub>H<sub>4</sub> conversion. The former is strongly wavelength-dependent, which mainly induces C<sub>2</sub>H<sub>4</sub> dehydrogenation into the C<sub>2</sub>H<sub>3</sub><sup>•</sup> radical, which follows an Eley–Rideal (E–R) type direct mechanism. Conversely, the latter induces two parallel reaction pathways to produce C<sub>2</sub>H<sub>2</sub> via the elimination pathway and acetaldehyde (CH<sub>3</sub>CHO) via the addition pathway. The latter pathway may undergo formation of oxometallacycle intermediates on the surface. These results not only achieve C<sub>2</sub>H<sub>4</sub> direct conversion into useful partial oxidation products via photocatalysis but also further deepen the understanding of the nature of C–H activation.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"39 12","pages":"5929–5937 5929–5937"},"PeriodicalIF":5.2,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143703863","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}