{"title":"Effects of Reduction Pretreatment on Ni─Cu Bimetallic Catalysts and Their Catalytic Performance on CO2 Hydrogenation","authors":"Qihang Wen, Yifei Feng, Haoyuan Gu, Haitao Yan, Zixu Yang, Minghui Zhu, Jing Xu","doi":"10.1002/ghg.2332","DOIUrl":"10.1002/ghg.2332","url":null,"abstract":"<div>\u0000 \u0000 <p>The performance of bimetallic catalysts is closely related to their surface structure, and the surface reconstruction process can affect the distribution of active sites, electronic structure, and reactant adsorption behavior. Traditional research has mostly focused on optimizing synthesis processes, such as controlling the size and distribution of metal particles, whereas there is relatively little research on the effect of pretreatment conditions on the dynamic structure of catalysts. In this study, a 10Ni─1Cu catalyst was synthesized using the deposition–precipitation method, and the effects of different pretreatment conditions on its performance were investigated. The catalyst was first pretreated at 500°C in a 60%H<sub>2</sub>/40%N<sub>2</sub> atmosphere, followed by reduction under different pretreatment atmospheres (10%H<sub>2</sub>/90%N<sub>2</sub> or 15%CO<sub>2</sub>/60%H<sub>2</sub>/25%N<sub>2</sub>) at the same temperature. At 400°C and a space velocity of 30 L h<sup>−1</sup> g<sup>−1</sup>, the methane production rate of the catalyst treated in the reaction atmosphere significantly increased from 12.4 to 15.8 µmol g<sup>−1</sup> s<sup>−1</sup> compared to the catalyst treated with hydrogen alone. Characterization techniques, such as TEM, x-ray photoelectron spectroscopy (XPS), and diffuse reflectance infrared Fourier transform spectroscopy (CO-DRIFTS), were employed to study the structural properties of the catalysts, focusing on the surface properties after reduction and the surface species during the reaction. This study demonstrates that catalysts pretreated in the reaction atmosphere enhance methane production rates by regulating the surface structure and forming Ni─Cu alloy structures with a lower Ni/Cu ratio, thereby optimizing the selectivity of hydrogenation products.</p>\u0000 </div>","PeriodicalId":12796,"journal":{"name":"Greenhouse Gases: Science and Technology","volume":"15 2","pages":"197-205"},"PeriodicalIF":2.8,"publicationDate":"2025-02-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143822221","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Slyvester Yew Wang Chai, Bing Shen How, Lock Hei Ngu
{"title":"Elucidation of Potable Water Accelerated Weathering of Limestone for Post-Combustion Carbon Capture: Correlation, Optimization, Comparative, Kinetic Modelling and Mass Transfer Analysis","authors":"Slyvester Yew Wang Chai, Bing Shen How, Lock Hei Ngu","doi":"10.1002/ghg.2329","DOIUrl":"10.1002/ghg.2329","url":null,"abstract":"<p>Energy generation and industrial processes are the main emitters of CO<sub>2</sub>, with 37.4 billion tCO<sub>2</sub> in 2023, causing detrimental environmental effects. As absorption is the most established carbon capture technology, this research implements the accelerated weathering of limestone (AWL) process to capture CO<sub>2</sub> from post-combustion emissions. However, this work replaces the conventional water source for the AWL process, seawater, with potable water. A correlation study was performed to study the effect of the proposed process's liquid-to-gas (L/G) ratio on the performance (i.e., effluent's alkalinity and CO<sub>2</sub> capture efficiency). The correlation findings show that by decreasing the L/G ratio (1–0.003), the calcium bicarbonate (Ca(HCO<sub>3</sub>)<sub>2</sub>) effluent concentration (0.77–3.65 mM) and pH (5.58–7.47) increase significantly, whereas CO<sub>2</sub> capture efficiency (81.94%–20.82%) was adversely affected. The optimization analysis obtained the highest achievable alkalinity at 3.63 mM at an optimized liquid and gas flow rate of 0.024 and 10 L min<sup>−1</sup>, respectively. Meanwhile, the liquid and gas flow rates of 1.23 and 1 L min<sup>−1</sup> achieved the highest CO<sub>2</sub> capture efficiency of 82.15%. It was deduced that potable water is better than seawater for CO<sub>2</sub> capture operation via the AWL process, achieving a 12.09%–39.14% better CO<sub>2</sub> capture efficiency when operated at similar conditions. In addition, the kinetic and mass transfer performance of the proposed process was also established in this work. Overall, this research establishes the potential of a potable water-operated AWL process for future commercialization.</p>","PeriodicalId":12796,"journal":{"name":"Greenhouse Gases: Science and Technology","volume":"15 2","pages":"178-196"},"PeriodicalIF":2.8,"publicationDate":"2025-02-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ghg.2329","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143822254","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yasaman Hosseinzadeh Dehaghani, Mehdi Assareh, Farzaneh Feyzi
{"title":"Molecular Dynamics Insights Into the Phase Equilibria and Thermophysical Properties of CO2–H2S–Brine System During Acid Gas Sequestration in Saline Aquifers","authors":"Yasaman Hosseinzadeh Dehaghani, Mehdi Assareh, Farzaneh Feyzi","doi":"10.1002/ghg.2327","DOIUrl":"10.1002/ghg.2327","url":null,"abstract":"<div>\u0000 \u0000 <p>This work represents an extensive molecular dynamics (MDs) simulation study with the microstructural insight at the interface to simultaneously predict the phase equilibria, transport, and interfacial properties of the CO<sub>2</sub>–H<sub>2</sub>S–brine system within the range of temperatures 323.15–393.15 K, pressures up to 30 MPa, H<sub>2</sub>S contents of 0–70 mol%, and salt molalities of 1–4 mol/kg, aiming to address the insufficiency of data under typical conditions of acid gas sequestration. The validation results demonstrate that the average absolute deviations (AAD%) for the predicted solubility of CO<sub>2</sub> and H<sub>2</sub>S in water and in 2 mol/kg NaCl solution were found to be 5.45%, 6.34%, 5.78%, and 5.41%, respectively. Moreover, the AAD% for interfacial tension (IFT) and density were 6.74% and 3.70%, respectively, verifying the validity and performance of the applied force field parameters and computational methods. The simulation results indicated that H<sub>2</sub>S solubility in brine is more sensitive to changes in the acid gas composition and temperature compared to CO<sub>2</sub> solubility. The presence of H<sub>2</sub>S remarkably reduces the CO<sub>2</sub>–H<sub>2</sub>S–brine IFT, with the reduction degree depending on the H<sub>2</sub>S content. Increasing the H<sub>2</sub>S mole fraction in acid gas mixtures delays convective mixing by reducing the brine density. At about 64 mol% H<sub>2</sub>S, the aqueous solution's density equals that of fresh brine, which is the highest H<sub>2</sub>S content that can maintain the benefit of convective mixing in the dissolution trapping. The maximum acid gas column height that can be safely stored is most significant at lower temperature and H<sub>2</sub>S content. On the basis of the results, pressure, temperature, and salt molality have a higher influence on the viscosity than density in the studied ranges. The new data generated by the current study can be utilized to develop predictive models of acid gas long-term behavior, which will reduce the uncertainty of real storage schemes.</p>\u0000 </div>","PeriodicalId":12796,"journal":{"name":"Greenhouse Gases: Science and Technology","volume":"15 2","pages":"154-177"},"PeriodicalIF":2.8,"publicationDate":"2025-02-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143822125","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Lin Wang, Jiabin Liu, Xiangjun Chen, Hanxiao Guo, Shuailong Feng
{"title":"Stress Distribution Characteristics Near Small Coal Faults and Prediction of Coal and Gas Outburst Risk","authors":"Lin Wang, Jiabin Liu, Xiangjun Chen, Hanxiao Guo, Shuailong Feng","doi":"10.1002/ghg.2331","DOIUrl":"10.1002/ghg.2331","url":null,"abstract":"<div>\u0000 \u0000 <p>This study aims to accurately predict the risk of coal and gas outbursts in coal seams located near small faults. Models of small-scale normal faults in the Changping mine field were constructed using the FLAC3D software, with fault dip angles of 65° and 70°, and drops of 1, 3, 5, 8, and 10 m. The objective was to analyze the effects of fault drop and dip angle on stress distribution near the faults and to predict the related outburst risks. The results indicate that in the hanging wall of the fault, the peak stress correlates with the fault drop through a linear function, whereas the range of influence is described by a quadratic function. As the fault drop increases, the impact range and stress peak also increase. The position of the stress peak gradually shifts away from the section, whereas the stress concentration area widens. Furthermore, the protruding danger zone expands and similarly moves farther from the section. When the fault drop is constant, the impact range of the 65° dip fault is smaller; however, the stress peak and the stress concentration zone in the nearby coal seam are larger and closer to the fault surface. Additionally, the highlighted danger zone is also larger and nearer to the fault surface. On the basis of the measured fundamental parameters of coal seam gas in the region, within a distance of 6 m from the fault surface (Zone I), there is a significant influence from the fault, resulting in a higher risk of outburst in this area. In the range of 6–15 m from the fault surface (Zone II), the gas content continues to increase, leading to an overall heightened risk of outburst.</p>\u0000 </div>","PeriodicalId":12796,"journal":{"name":"Greenhouse Gases: Science and Technology","volume":"15 2","pages":"142-153"},"PeriodicalIF":2.8,"publicationDate":"2025-02-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143822066","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Emad Ansari Ardehjani, Mohammad Ataei, Farhang Sereshki, Ali Mirzaghorbanali, Naj Aziz
{"title":"Impact of Diverse Parameters on CO2 Adsorption in CO2 Sequestration: Utilizing a Novel Triaxial Testing Apparatus","authors":"Emad Ansari Ardehjani, Mohammad Ataei, Farhang Sereshki, Ali Mirzaghorbanali, Naj Aziz","doi":"10.1002/ghg.2322","DOIUrl":"10.1002/ghg.2322","url":null,"abstract":"<div>\u0000 \u0000 <p>In order to minimize greenhouse gas emissions, it is essential from an environmental point of view to employ CO<sub>2</sub> sequestration technology to store CO<sub>2</sub> in underground coal layers. To study this strategy, a triaxial testing apparatus is required. This study introduces a novel triaxial testing apparatus developed to explore enhanced coal bed methane (ECBM) and carbon dioxide (CO<sub>2</sub>) sequestration techniques. Several laboratory tests were conducted to validate the apparatus and study the behavior of coal exposed to CO<sub>2</sub> using this machine. In fact, the implementation of this machine marks the initial step in an empirical feasibility analysis of CO<sub>2</sub> sequestration in Iranian coal seams. This analysis involves examining the impact of ash content, ambient temperature, and saturation direction on CO<sub>2</sub> adsorption and emission in various coal samples. Two different thermal coal samples from Chamestan and Tash mines were utilized. Some results, such as the trend of the coal sample's strain, show good correlation with previous work. Additionally, some results presented in this work are novel. On the basis of the results, the developed apparatus demonstrated satisfactory performance, and its innovative design fully meets the desired outcome. Higher ash content increases coal strength and reduces deformation. Lower ash content leads to more gas adsorption and deformation post-saturation. Gas adsorption is higher at 25°C than at 4°C. Moreover, coal samples at 25°C had 12.5 times more axial strain than those at 4°C. Lateral saturation causes 13.72% larger axial strain changes than top and end saturation due to increased gas-sample contact and penetration into the coal matrix.</p>\u0000 </div>","PeriodicalId":12796,"journal":{"name":"Greenhouse Gases: Science and Technology","volume":"15 1","pages":"53-67"},"PeriodicalIF":2.8,"publicationDate":"2025-01-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143381066","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Research Progress on CO2 Geological Storage Reservoir and Caprock Mechanics: Methods and Status","authors":"Shuaiyi Lu, Pan Jiang, Lianghan Cong, Xiaoshu Lü","doi":"10.1002/ghg.2328","DOIUrl":"10.1002/ghg.2328","url":null,"abstract":"<div>\u0000 \u0000 <p>Greenhouse gas (GHG) emissions have caused serious global climate change, and countries worldwide are taking steps to mitigate the greenhouse effect caused by carbon emissions. CO<sub>2</sub> geological storage (CGS) is emerging as a large-scale technology for reducing GHG emissions and is gradually becoming one of the most important means of mitigating the greenhouse effect. There are several problems in the implementation of this technology, among which the geomechanical problems caused by injection sequestration cannot be ignored. This article reviews the impacts and hazards of geomechanical problems caused by injection and sequestration in CGS, which can lead to risks, including changes in reservoir and caprock mechanical properties, reservoir stability, caprock closure, fault activation, and induced seismicity during CO<sub>2</sub> injection and sequestration. This article reviews the above studies and summarizes the research methods of CGS geomechanical problems and generation mechanisms, which can help to comprehensively understand the risks faced in the CGS process and provide references and guidance for the operation, monitoring, and research of CGS in the future.</p>\u0000 </div>","PeriodicalId":12796,"journal":{"name":"Greenhouse Gases: Science and Technology","volume":"15 2","pages":"264-276"},"PeriodicalIF":2.8,"publicationDate":"2025-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143822198","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Nickel Aluminum Spinel Derived Ni-F-Al Active Site for the Catalytic Dehydrofluorination of Potent Greenhouse Gas 1,1,1,2-Tetrafluoroethane","authors":"Fangcao Liu, Bing Liu, Yiwei Sun, Jinru Liu, Yubao Bi, Jiaming Zhao, Xiaoli Wei, Wenfeng Han","doi":"10.1002/ghg.2324","DOIUrl":"10.1002/ghg.2324","url":null,"abstract":"<div>\u0000 \u0000 <p>HFC-134a (1,1,1,2-tetrafluoroethane) is one of the most common refrigerants with global warming potential (100 years) of 1300. It is regulated to be phased out gradually according to the Kigali Amendment to the Montreal Protocol. Treatment of this stable chemical poses significant challenge. Highly efficient nickel aluminum spinel catalysts were fabricated by sol–gel method for the catalytic dehydrofluorination of HFC-134a. The effect of Ni/Al ratio in the NiAl<sub>2</sub>O<sub>4</sub> spinel precursors on the performance of NiAl catalysts was studied by x-ray diffraction (XRD), Brunauer–Emmett–Teller (BET), scanning electron microscope (SEM), transmission electron microscopy (TEM), NH<sub>3</sub>-TPD, and XPS. Nickel–aluminum ratio in the nickel–aluminum spinel precursor plays a major role on the formation of strong acid and active species Ni-F-Al. With Ni/Al ratio of 4, the (3 1 1) crystal face of NiAl<sub>2</sub>O<sub>4</sub> interfaced with the (1 1 1) crystal face of NiO and the (4 0 0) crystal face of NiAl<sub>2</sub>O<sub>4</sub>. This interaction facilitates the formation of Ni-F-Al active species following the dehydrofluorination reaction. Furthermore, the Ni-F-Al species altered the acid structure of NiAl catalysts. It was found that NiAl catalyst with a Ni/Al ratio of 4 has the best catalytic performance compared with other catalysts (with conversion of 35%), and no deactivation trend was observed after 50 h of time on stream. (Reaction conditions: N<sub>2</sub>/CF<sub>3</sub>CH<sub>2</sub>F = 10, T = 450°C, GHSV = 660 h<sup>−1</sup>).</p>\u0000 </div>","PeriodicalId":12796,"journal":{"name":"Greenhouse Gases: Science and Technology","volume":"15 1","pages":"68-78"},"PeriodicalIF":2.8,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143380938","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}