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American Chemical Society
Energy & fuels

American Chemical Society

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0887-0624

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    Canada's Hydrogen Future: Innovations, Policies, and Global Perspectives

    Bahrain GhorbaniSohrab ZendehboudiNoori M. Cata SaadyGreg F. Naterer...
    7605-7648页
    查看更多>>摘要：Canada has the essential elements to develop a sustainable hydrogen (H_2) economy, including abundant feedstock, a strong energy sector, and international partnerships. The country's climate commitments, financial incentives, and expertise position it as a leader in pursuing net-zero goals. However, a comprehensive framework is needed to integrate H_2 storage technologies, industrial applications, research and development (R&D), regulations, and international collaborations. This review paper presents a detailed assessment of H_2 storage methods, their applications, and key end-users in Canada. The application across various domains is examined in detail, including its role as a fuel (e.g., electricity generation and transportation), a heat source (e.g., buildings and industrial processes), and a feedstock (e.g., the oil and gas sectors and synthetic fuel production). The regulatory and policy frameworks that shape Canada's H_2 economy are analyzed, with a focus on key initiatives, funding programs, and their associated opportunities and challenges. R&D needs are highlighted, focusing on current R&D activities, key priorities, and areas for future investments. The contributions of public-private partnerships in advancing H_2 R&D in conjunction with contributions from research centers and universities across Canada are considered. Key findings and insights are categorized, and the prospects for H_2 energy in Canada's future are discussed. Recommendations are provided for policymakers, industry stakeholders, and researchers to support the continued development and implementation of H_2 energy solutions. In addition, the strategies and objectives of the H_2 short-, medium-, and long-term plans are presented with highlights of the provincial strategies. International collaborations and case studies are discussed, and insights into global practices and their applications in Canada are provided.
      原文链接:
    • NETL
    • NSTL
    • Amer Chemical Soc

    Rational Design of Catalytically Active Sites in Metal-Free Carbon Materials for Electrocatalytic CO_2 Reduction: A Review

    Shaoqin ChenYun Hang Hu
    7649-7664页
    查看更多>>摘要：Electrocatalytic conversion of carbon dioxide (CO_2) into value-added chemicals is a promising avenue for reducing greenhouse gas emissions while storing renewable energy in its chemical form. Metal-free carbon-based materials have attracted growing interest as electrocatalysts for CO_2 reduction due to their abundance, low cost, stability, and tunable electronic structures. However, pristine carbon materials, such as graphene, lack catalytic activity due to the weak physisorption of CO_2, necessitating the creation of active sites to boost electrocatalytic performance. In this review, we highlight recent advances in tailoring carbon frameworks through two key strategies to enhance the performance of electrocatalytic CO_2 reduction. The first strategy, heteroatom doping-including nitrogen, phosphorus, boron, and fluorine-creates localized electronic states that direct reaction pathways toward specific products. The second strategy involves engineering defects, such as vacancies or pentagonal/octagonal ring structures, which significantly boost local electron density and adsorbate binding affinity, thereby lowering CO_2 activation barriers. By creating these active sites, the electrocatalytic performance of carbon materials can be enhanced by over 2 orders of magnitude compared with inert carbon. Additionally, mechanistic insights from both experimental and computational studies are discussed, illustrating how electronic reconfiguration, spin density, and local coordination environments govern catalytic activity and selectivity. Finally, we outline challenges and future research directions for achieving sustainable CO_2 electroreduction.
      原文链接:
    • NETL
    • NSTL
    • Amer Chemical Soc

    Safety Hazards of Lithium Metal Batteries: From the Perspective of Lithium Dendrites and Thermal Runaway

    Xiangming CuiJingzhao WangShiyi SunXin Chen...
    7665-7690页
    查看更多>>摘要：Lithium metal batteries (LMBs) have stepped into the spotlight for a decade, featuring significant potential for high energy density as well as compatibility with off-the-shelf lithium-ion technologies. However, the commercialization of LMBs has lagged behind expectations due to safety concerns related to short circuits. Recent advancements have focused on tackling lithium dendrites and separator/electrolyte-related dielectric failure. In this review, we cover the main factors that promote lithium dendrites and cause separator/ electrolyte failure, highlighting the lithium plating mechanism and the decomposition chain triggered by Joule heat. Based on the fundamentals of electrochemistry, we assess and summarize the promising approaches that have been widely applied and proven in literature practice, including the construction of separators with high mechanical modulus and lithium affinity, the incorporation of functional components in electrolytes to regulate lithium plating, and the enhancement of the thermal stability and thermal strain ability of the separator/electrolyte system, among others. We believe that the understanding of mechanisms and proposed strategies may approach the threshold of breakthroughs, and a periodical review is helpful for both academia and industry in pursuing the commercialization of LMBs.
      原文链接:
    • NETL
    • NSTL
    • Amer Chemical Soc

    Recent Advances in Cerium-Based Catalysts for NO Reduction by CO: A Review

    Pengyu DuChuanmin ChenXianghongyang ChenYue Cao...
    7691-7712页
    查看更多>>摘要：Nitrogen oxides (NO_x) are a significant component of air pollutants, and research on denitrification (de-NO_x) catalysts has become relatively mature. However, in specific fields, such as industrial production and vehicle operation, exhaust also primarily contains carbon monoxide (CO). CO selective catalytic reduction (CO-SCR) effectively eliminates NO_x from flue gases while converting CO into non-toxic carbon dioxide (CO_2). Although Ce-based catalysts are a major focus of research in de-NO_x treatment, there is a lack of comprehensive reviews on their application in CO reduction of NO. This review examines the reaction mechanisms of CO-SCR and evaluates the catalytic performance of various Ce-based catalysts within the current research framework. Both catalysts with Ce-based active components and supported cerium-based catalysts showed superior performance, with NO conversion rates typically exceeding 90% and complete CO conversion at approximately 300 ℃. This review examines catalyst chemical poisoning and outlines the deactivation causes of Ce-based catalysts when exposed to oxygen, water vapor, and sulfur dioxide. It also proposes corresponding mitigation strategies. On this basis, some suggestions for future research on industrial flue gas denitrification are proposed. This review seeks to offer insights for the industrial use of CO-SCR catalysts.
      原文链接:
    • NETL
    • NSTL
    • Amer Chemical Soc

    Synthesis and Application of Time-Gated Fluorescent Tags for Tracing Downhole Fluids and Mineral Samples

    Marta AntonivS. Sherry ZhuGawain ThomasMartin E. Poitzsch...
    7713-7722页
    查看更多>>摘要：We have developed a nanoparticle (NP) composed of a polystyrene-vinyl benzoic acid copolymer via one-pot emulsion polymerization. This NP anchors a Eu~(3+) complex with a 1,10- phenanthroline antenna ligand (PS-VBA-Eu-Phen). With only 15 mol % of the Eu~(3+) ion relative to styrene, this low-cost and readily scalable NP exhibits the characteristic luminescence of ligand-to- metal charge transfer from the Eu~(3+) complex. We determined the lifetime and the intrinsic quantum yield of the strongest ~5D_0 → ~7F_2 luminescence for the Eu~(3+) complex inside the NPs. The long lifetime of the luminescence ensures clear detection of the PS-VBA-Eu-Phen NPs in complex oil-based mud (OBM) and on mineral samples (cuttings) recovered from the OBM using time-gated emission measurement. This method effectively reduces the background emission from minerals or additives in the mud and promises potential applications of the NP as a tracer or tag for tracking downhole fluids and cuttings.
      原文链接:
    • NETL
    • NSTL
    • Amer Chemical Soc

    Gas Production Optimization from 3D Hydrate Dissociation via Depressurization in Multiply Fractured Reservoirs

    Li ZhangQingping LiRanjith P. GamageBisheng Wu...
    7723-7738页
    查看更多>>摘要：Natural gas hydrate (NGH), a clean energy resource with vast reserves and high energy density, holds significant potential to address global energy demands. However, its commercial exploitation remains challenging due to low dissociation efficiency under conventional extraction methods. To address this limitation, this study investigates the synergistic effects of hydraulic fracturing and depressurization on enhancing NGH mining. A three-dimensional model is developed using the commercial package, TOUGH + HYDRATE, to study the NGH dissociation by depressurization from a single horizontal well intercepted by multiple hydraulic fractures. After a sensitivity analysis is carried out, a quantitative relationship between the fracture density (N_d), depressurization amplitude (P_w) and the gas production performance is established. The results reveal that the dissociation rate in the case with fractures is several orders of magnitude higher than that in the case without fractures. Notably, the impact of N_d on production diminishes at higher N_d values. Increasing N_d from 1 to 3 enhances cumulative gas release by over 30%, whereas further increases to N_d = 4 and 5 yield only about 18% incremental gains. Additionally, at small depressurization amplitudes (P_w = 0.8P_0—0.9P_0), fracture density exerts minimal influence on dissociation efficiency due to insufficient driving forces. Spatial analysis shows that dissociation fronts initially form and propagate near the wellbore, but later exhibit near the upper and lower boundaries of the NGH layer. The gas distribution gradually increases during the initial year, but subsequently concentrates only near advancing fronts, driven by fluid influx from adjacent strata and the presence of high-permeability flow channels. These findings demonstrate that optimizing fracture density and depressurization amplitude is critical for balancing extraction efficiency, providing actionable insights for designing field-scale NGH production strategies.
      原文链接:
    • NETL
    • NSTL
    • Amer Chemical Soc

    Thermal Evolution of Organic Matter in Low-Maturity Shale: A Multimodal Nanoscale Investigation

    Yingjie LiTianhao WuJunliang ZhaoGuorui Wang...
    7739-7750页
    查看更多>>摘要：Systematic characterization of the nanoscale geomechanical and geochemical evolution of organic matter at elevated temperatures is critical for assessing the technical feasibility of in situ thermal methods in the development of low-maturity shale oil and gas. This study investigates the pyrolysis process of low-maturity, organic-rich shale from Yanchang Formation, focusing on thermal evolution in morphology, geochemistry, and geomechanical properties. The comprehensive analysis is performed through a series of sophisticated techniques, including thermogravimetric analysis coupled with thermogravimetric-Fourier transform infrared-gas chromatography/mass spectrometry (TG-FTIR-GC/MS), backscattered electron of the scanning electron microscopy (BSE-SEM), micro-Raman spectroscopy, atomic force microscopy-infrared spectroscopy (AFM-IR), and AFM PeakForce quantitative nanomechanics (PFQNM). Pyrolysis products evolve across three stages: water vapor dominates below 200 ℃; hydrocarbons, CO_2, and sulfur compounds release in the range of 200-650 ℃; and carbonate decomposition drives CO_2 emissions above 650 ℃. Heating induces significant morphological alterations, including surface shrinkage, pore collapse, and thermal cracks (notably above 400 ℃). Geochemical analyses show that the differences in structure among solid bitumen, vitrinite, and inertinite decrease as the temperature increases, alongside detaching aliphatic side chains and oxygenated functional groups and increasing the degree of aromatization. Geomechanical properties, measured via AFM-PFQNM, demonstrate an initial decrease in Young's modulus (25-250 ℃) due to pore water loss, followed by modulus increase (250-600 ℃) attributed to the aromaticity enhancement and matrix shrinkage. These insights advance the understanding of in situ thermal conversion processes, offering practical guidelines for enhancing hydrocarbon recovery from low-maturity shale reservoirs. The multidisciplinary approaches resolve the interplay among thermal, chemical, and mechanical dynamics in shale pyrolysis.
      原文链接:
    • NETL
    • NSTL
    • Amer Chemical Soc

    Separate Classification Prediction Model for Lithofacies Identification of Paleogene Yingxiongling Shale, Qaidam Basin

    Yue ShenSongtao WuYinghao ShenKunyu Wu...
    7751-7765页
    查看更多>>摘要：Abundant shale oil resources have been discovered in the upper member of the Paleogene Lower Ganchaigou Formation of the Yingxiongling area from the Qaidam Basin, China. The lithofacies of Yingxiongling shale oil exhibit strong heterogeneity vertically. Accurate lithofacies identification is the key to characterizing the potential of unconventional oil and gas resources. Traditional lithofacies identification is limited by factors such as the duration of experiments and the subjectivity of the scholars. Only a limited amount of coring section data is available for analysis, while a sea of logging data remains underutilized. Therefore, utilizing machine learning algorithms to effectively leverage logging data for constructing the accurate lithofacies identification model has become a crucial area in both academia and industry. In this paper, 15 basic logging curves were used, and algorithms of random forest (RF), support vector machine (SVM), and extreme gradient boosting (XGBoost) were selected through Python programming to establish machine learning classification models, identifying the lithofacies types of Yingxiongling shale and analyzing the results. The lithofacies classification scheme of Yingxiongling shale is based on "rock structure + mineral composition", developing 8 lithofacies types: thin-bedded/ laminated dolomitic limestone, thin-bedded/laminated limy dolostone, thin-bedded sandstone, laminated shale, and thin-bedded/ laminated mixed rock. Due to the differing sensitivities of various logging data in identifying rock structures and mineral compositions, the corresponding algorithms and parameters vary accordingly. Hence, an innovative stepwise prediction model integrating "sedimentary structures and mineral composition" is proposed. The model first identified the rock structure through the genetic algorithm-RF and 15 logging curves, yielding thin-bedded/laminated structures. Then, SVM and 9 logging curves were used to identify mineral composition, yielding limy dolostone, dolomitic limestone, sandstone, shale, and mixed rock. The lithofacies were obtained by integrating the predicted results from the two models. The maximum accuracy of identifying rock structure and mineral composition can reach 87.3% and 78.7%, respectively, and the maximum prediction accuracy of the separate prediction model reached 73.2%, which is 22% higher than that of the direct prediction model. The relationship between the well logging curves and the predicted results is discussed, and the reasons for errors will be explained. These understandings can further help provide new ideas and methods for the identification of shale lithofacies types and can provide scientific guidance and technical support for the exploration and development of the Qaidam Basin.
      原文链接:
    • NETL
    • NSTL
    • Amer Chemical Soc

    Influence of Polyvinylpyrrolidone and Cassava Starch on the Formation Kinetics of CO_2 Hydrate

    Nan LiXucheng DongJingkai XuJingchen Liu...
    7766-7780页
    查看更多>>摘要：CO_2 hydrate blockages may occur in the application of CO_2 capture, utilization, and storage (CCUS). Under specific conditions, CO_2 hydrates exhibit great stability and pose significant challenges in prevention and control. Current research primarily focuses on the prevention of natural gas hydrates, while research on the prevention of CO_2 hydrates is relatively limited. In this work, the formation kinetics of CO_2 hydrates in the presence of two kinetic inhibitors, polyvinylpyrrolidone (PVP) and cassava starch, were investigated. Effects of subcooling, inhibitor concentrations, inhibitor molecular weights, and compositions of the mixture of PVP and starch were considered. The results indicate that at subcooling lower than 6.2 K (2.5 MPa, 272.95 K), 1 wt % PVP-K32 can exhibit good inhibition effect. Cassava starch has a better inhibition effect than PVP, with concentration of 0.2-0.5 wt %, it can effectively inhibit the hydrate formation for more than 6 h at the subcooling of 6.2K (2.5 MPa, 272.95 K). Inhibitor blend (1 wt % PVP-K32 + 1 wt % cassava starch) demonstrates good inhibition performance at the high subcooling of 8.9 K (3.5 MPa, 272.95 K). A significant concentration effect was observed. Under the supercooling of 8.9 K, PVP-K32 can delay the nucleation of hydrates, but its inhibitory effect on the growth process of the hydrates became weak with the increase of concentration. CO_2 hydrates exhibited a distinct interface growth phenomenon, forming thin films that act as a barrier to mass transfer. Stable hydrate films along with kinetic inhibitors inhibited the nucleation and growth of hydrates. However, under high turbulence conditions, this inhibitory effect is significantly weakened. In addition, sheet-like or vein-like hydrates morphologies were also observed in the presence of inhibitors. These results can provide support for the development of kinetic inhibitors for CO_2 hydrates to address hydrate blockage issues in Correlated engineering.
      原文链接:
    • NETL
    • NSTL
    • Amer Chemical Soc

    Enhancement of Biogenic Coalbed Methane by ScCO_2-H_2O Treatment

    Xiyang FengLunru YanHongguang GuoZaixing Huang...
    7781-7789页
    查看更多>>摘要：Supercritical CO_2 (ScCO_2) extraction could enhance biogenic methane production from coal by optimizing the coal structure, and water acted as an entrainer to improve the extraction efficiency of ScCO_2. In this study, the methane production experiments were conducted on anthracite with different moisture contents treated with ScCO_2. The changes in coal structure, organic matter, and elemental content caused by ScCO_2-H_2O treatment were analyzed. The methane production increased by 46.1 % as moisture content rose from 0% to 20%, but did not continue to increase at 30% due to nutrient leaching. Under water-immersed conditions, although the methane production from ScCO_2 treated coal decreased, the total methane production from ScCO_2 treated coal and leachate reached 314.95 μmol/g coal. This value was increased by 61.59% compared with that of raw coal. These findings highlighted the dual role of moisture in facilitating ScCO_2 extraction and shifting methane generation from coal to leachate. Structural analysis confirmed that moisture enhanced the effect of ScCO_2 on functional groups in coal. Specifically, the total amount of aromatics with two substitutions and aromatics with three substitutions decreased progressively from 67.98% to 54.27% with increasing moisture content. The same phenomenon was also observed for carboxylic acids and C=O functional groups with maximum reductions of 100% and 71.51%. Instead, the CH_3/CH_2 ratio was positively correlated with moisture content. The concentrations of TOC, straight-chain alkanes, iron, nickel, and cobalt in leachate treated with ScCO_2-H_2O increased by 5.52, 1.35, 11 592.79, 229.17, and 27.76 times, respectively, compared to those in leachate treated with water alone, supporting the high methane production in leachate. It highlighted that moisture-driven structural modifications and nutrient mobilization were key mechanisms for optimizing the enhancement of ScCO_2 on microbially enhanced coalbed methane (MECBM). These findings suggested that water-bearing anthracite coal seam would be a suitable stratum for ScCO_2 enhanced MECBM.
      原文链接:
    • NETL
    • NSTL
    • Amer Chemical Soc