Ammonia is an exceptional fuel for solid oxide fuel cells (SOFCs), because of the high content of hydrogen and the advantages of carbon neutrality. However, the challenge lies in its unsatisfactory performance at intermediate temperatures (500–600 °C), impeding its advancement. An electrolyte-supported proton-ceramic fuel cell (PCFC) was fabricated employing BaZr0.1Ce0.7Y0.2O3−δ (BZCY) as the electrolyte and Ba0.5Sr0.5Co0.8Fe0.2O3−δ (BSCF) as the cathode. In this study, the performance of PCFC using NH3 as fuel within an operating temperature range of 500–700 °C was improved by adding an M(Ni,Ru)/CeO2 catalyst layer to reconstruct the anode surface. The electrochemical performance of direct ammonia PCFC (DA-PCFC) were improved to different extents. Compared to H2 as fuel, the degradation ratio of peak power densities (PPDs) of Ni/CeO2-loaded PCFC fueled with NH3 decreased at 700–500 °C, with a decrease to 13.3% at 700 °C and 30.7% at 500 °C. The findings indicate that Ru-based catalysts have a greater promise for direct ammonia SOFCs (DA-SOFCs) at operating temperatures below 600 °C. However, the enhancement effect becomes less significant above 600 °C when compared to Ni-based catalysts.
{"title":"Performance-enhanced direct ammonia protonic ceramic fuel cells using CeO2-supported Ni and Ru catalyst layer","authors":"Xiaoxiao Li, Jiangping Chen, Yunyun Huang, Huihuang Fang, Chongqi Chen, Fulan Zhong, Li Lin, Yu Luo, Yuqing Wang, Lilong Jiang","doi":"10.1007/s11708-024-0959-z","DOIUrl":"10.1007/s11708-024-0959-z","url":null,"abstract":"<div><p>Ammonia is an exceptional fuel for solid oxide fuel cells (SOFCs), because of the high content of hydrogen and the advantages of carbon neutrality. However, the challenge lies in its unsatisfactory performance at intermediate temperatures (500–600 °C), impeding its advancement. An electrolyte-supported proton-ceramic fuel cell (PCFC) was fabricated employing BaZr<sub>0.1</sub>Ce<sub>0.7</sub>Y<sub>0.2</sub>O<sub>3−δ</sub> (BZCY) as the electrolyte and Ba<sub>0.5</sub>Sr<sub>0.5</sub>Co<sub>0.8</sub>Fe<sub>0.2</sub>O<sub>3−δ</sub> (BSCF) as the cathode. In this study, the performance of PCFC using NH<sub>3</sub> as fuel within an operating temperature range of 500–700 °C was improved by adding an M(Ni,Ru)/CeO<sub>2</sub> catalyst layer to reconstruct the anode surface. The electrochemical performance of direct ammonia PCFC (DA-PCFC) were improved to different extents. Compared to H<sub>2</sub> as fuel, the degradation ratio of peak power densities (PPDs) of Ni/CeO<sub>2</sub>-loaded PCFC fueled with NH<sub>3</sub> decreased at 700–500 °C, with a decrease to 13.3% at 700 °C and 30.7% at 500 °C. The findings indicate that Ru-based catalysts have a greater promise for direct ammonia SOFCs (DA-SOFCs) at operating temperatures below 600 °C. However, the enhancement effect becomes less significant above 600 °C when compared to Ni-based catalysts.</p></div>","PeriodicalId":570,"journal":{"name":"Frontiers in Energy","volume":"18 6","pages":"875 - 884"},"PeriodicalIF":3.1,"publicationDate":"2024-08-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142175165","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-08-15DOI: 10.1007/s11708-024-0958-0
Shaoshan Xu, Xingchen Wu, Jun Shen, Haochen Hua
In the park-level integrated energy system (PIES) trading market involving various heterogeneous energy sources, the traditional vertically integrated market trading structure struggles to reveal the interactions and collaborative relationships between energy stations and users, posing challenges to the economic and low-carbon operation of the system. To address this issue, a dual-layer optimization strategy for energy station-user, taking into account the demand response for electricity and thermal, is proposed in this paper. The upper layer, represented by energy stations, makes decisions on variables such as the electricity and heat prices sold to users, as well as the output plans of energy supply equipment and the operational status of battery energy storage. The lower layer, comprising users, determines their own electricity and heat demand through demand response. Subsequently, a combination of differential evolution and quadratic programming (DE-QP) is employed to solve the interactive strategies between energy stations and users. The simulation results indicate that, compared to the traditional vertically integrated structure, the strategy proposed in this paper increases the revenue of energy stations and the consumer surplus of users by 5.09% and 2.46%, respectively.
{"title":"Low-carbon collaborative dual-layer optimization for energy station considering joint electricity and heat demand response","authors":"Shaoshan Xu, Xingchen Wu, Jun Shen, Haochen Hua","doi":"10.1007/s11708-024-0958-0","DOIUrl":"10.1007/s11708-024-0958-0","url":null,"abstract":"<div><p>In the park-level integrated energy system (PIES) trading market involving various heterogeneous energy sources, the traditional vertically integrated market trading structure struggles to reveal the interactions and collaborative relationships between energy stations and users, posing challenges to the economic and low-carbon operation of the system. To address this issue, a dual-layer optimization strategy for energy station-user, taking into account the demand response for electricity and thermal, is proposed in this paper. The upper layer, represented by energy stations, makes decisions on variables such as the electricity and heat prices sold to users, as well as the output plans of energy supply equipment and the operational status of battery energy storage. The lower layer, comprising users, determines their own electricity and heat demand through demand response. Subsequently, a combination of differential evolution and quadratic programming (DE-QP) is employed to solve the interactive strategies between energy stations and users. The simulation results indicate that, compared to the traditional vertically integrated structure, the strategy proposed in this paper increases the revenue of energy stations and the consumer surplus of users by 5.09% and 2.46%, respectively.</p></div>","PeriodicalId":570,"journal":{"name":"Frontiers in Energy","volume":"19 1","pages":"100 - 113"},"PeriodicalIF":3.1,"publicationDate":"2024-08-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142175143","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-08-10DOI: 10.1007/s11708-024-0955-3
Yanbo Wang, Tiankuo Chu
The frame of membrane electrode assembly (MEA) influences the durability of proton exchange membrane fuel cell (PEMFC). In this paper, the thermal shock bench was applied as an accelerated aging test to explore the effect of frame sealing structure on MEA durability at different temperatures. Analysis of scanning electron microscope (SEM) images reveals that thermal shock results in the formation of cracks on the exposed proton exchange membrane (PEM) at the gap between the frame and the active area. Moreover, it breaks the bonding interface between the frame and the membrane and leads to the debonding of the adhesive, which exacerbates the risk of crossover of the reactant gas. A comparison of the single-layer and improved double-layer frame structures reveal that the mechanical damage is caused by frequent membrane wrinkles in the gap under temperature shock. However, addition of a cushion layer improves the continuity between the frame and the active area, and reduces deformation of the membrane, thereby preventing membrane damage.
{"title":"Improvement of durability of membrane electrode assembly by frame sealing structure in temperature shock","authors":"Yanbo Wang, Tiankuo Chu","doi":"10.1007/s11708-024-0955-3","DOIUrl":"10.1007/s11708-024-0955-3","url":null,"abstract":"<div><p>The frame of membrane electrode assembly (MEA) influences the durability of proton exchange membrane fuel cell (PEMFC). In this paper, the thermal shock bench was applied as an accelerated aging test to explore the effect of frame sealing structure on MEA durability at different temperatures. Analysis of scanning electron microscope (SEM) images reveals that thermal shock results in the formation of cracks on the exposed proton exchange membrane (PEM) at the gap between the frame and the active area. Moreover, it breaks the bonding interface between the frame and the membrane and leads to the debonding of the adhesive, which exacerbates the risk of crossover of the reactant gas. A comparison of the single-layer and improved double-layer frame structures reveal that the mechanical damage is caused by frequent membrane wrinkles in the gap under temperature shock. However, addition of a cushion layer improves the continuity between the frame and the active area, and reduces deformation of the membrane, thereby preventing membrane damage.</p></div>","PeriodicalId":570,"journal":{"name":"Frontiers in Energy","volume":"19 3","pages":"326 - 333"},"PeriodicalIF":6.2,"publicationDate":"2024-08-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141921128","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-08-10DOI: 10.1007/s11708-024-0956-2
Yuan Zhao, Quan Wang, Rongrong Hu, Wenqiang Liu, Xiaojuan Zhang, Wei Wang, Nicolas Alonso-Vante, Dongdong Zhu
Fe-N-C catalysts are potential substitutes to displace electrocatalysts containing noble chemical elements in the oxygen reduction reaction (ORR). However, their application is hampered by unsatisfactory activity and stability issues. The structures and morphologies of Fe-N-C catalysts have been found to be crucial for the number of active sites and local bonding structures. In this work, dicyandiamide (DCDA) and polyaniline (PANI) are shown to act as dual nitrogen sources to tune the morphology and structure of the catalyst and facilitate the ORR process. The dual nitrogen sources not only increase the amount of nitrogen doping atoms in the electrocatalytic Fe-C-N material, but also maintain a high nitrogen-pyrrole/nitrogen-graphitic: (N-P)/(N-G) value, improving the distribution density of catalytic active sites in the material. With a high surface area and amount of N-doping, the Fe-N-C catalyst developed can achieve an improved half-wave potential of 0.886 V (vs. RHE) in alkaline medium, and a better stability and methanol resistance than commercial Pt/C catalyst.
{"title":"Oxygen reduction reaction performance of Fe-N-C catalyst with dual nitrogen source","authors":"Yuan Zhao, Quan Wang, Rongrong Hu, Wenqiang Liu, Xiaojuan Zhang, Wei Wang, Nicolas Alonso-Vante, Dongdong Zhu","doi":"10.1007/s11708-024-0956-2","DOIUrl":"10.1007/s11708-024-0956-2","url":null,"abstract":"<div><p>Fe-N-C catalysts are potential substitutes to displace electrocatalysts containing noble chemical elements in the oxygen reduction reaction (ORR). However, their application is hampered by unsatisfactory activity and stability issues. The structures and morphologies of Fe-N-C catalysts have been found to be crucial for the number of active sites and local bonding structures. In this work, dicyandiamide (DCDA) and polyaniline (PANI) are shown to act as dual nitrogen sources to tune the morphology and structure of the catalyst and facilitate the ORR process. The dual nitrogen sources not only increase the amount of nitrogen doping atoms in the electrocatalytic Fe-C-N material, but also maintain a high nitrogen-pyrrole/nitrogen-graphitic: (N-P)/(N-G) value, improving the distribution density of catalytic active sites in the material. With a high surface area and amount of N-doping, the Fe-N-C catalyst developed can achieve an improved half-wave potential of 0.886 V (vs. RHE) in alkaline medium, and a better stability and methanol resistance than commercial Pt/C catalyst.</p></div>","PeriodicalId":570,"journal":{"name":"Frontiers in Energy","volume":"18 6","pages":"841 - 849"},"PeriodicalIF":3.1,"publicationDate":"2024-08-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142175164","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-07-20DOI: 10.1007/s11708-024-0954-4
Muhammad Salman Nasir, Hu Pan, Baowen Zhou
{"title":"Economically attractive production of commercial-grade gasoline from waste plastics","authors":"Muhammad Salman Nasir, Hu Pan, Baowen Zhou","doi":"10.1007/s11708-024-0954-4","DOIUrl":"10.1007/s11708-024-0954-4","url":null,"abstract":"","PeriodicalId":570,"journal":{"name":"Frontiers in Energy","volume":"18 5","pages":"712 - 715"},"PeriodicalIF":3.1,"publicationDate":"2024-07-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141819550","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-07-15DOI: 10.1007/s11708-024-0951-7
Jianbo Tang, Bo Yuan, Hongzhang Wang, Jing Liu
{"title":"Visualizing unleashed latent heat of liquid metal for soft intelligence","authors":"Jianbo Tang, Bo Yuan, Hongzhang Wang, Jing Liu","doi":"10.1007/s11708-024-0951-7","DOIUrl":"10.1007/s11708-024-0951-7","url":null,"abstract":"","PeriodicalId":570,"journal":{"name":"Frontiers in Energy","volume":"18 5","pages":"545 - 549"},"PeriodicalIF":3.1,"publicationDate":"2024-07-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141648440","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The undesired side reactions at electrode/electrolyte interface as well as the irreversible phase evolution during electrochemical cycling significantly affect the cyclic performances of nickel-rich NMCs electrode materials. Electrolyte optimization is an effective approach to suppress such an adverse side reaction, thereby enhancing the electrochemical properties. Herein, a novel boron-based film forming additive, tris(2,2,2-trifluoroethyl) borate (TTFEB), has been introduced to regulate the interphasial chemistry of LiNi0.8Mn0.1Co0.1O2 (NMC811) cathode to improve its long-term cyclability and rate properties. The results of multi-model diagnostic study reveal that formation lithium fluoride (LiF)-rich and boron (B) containing cathode electrolyte interphase (CEI) not only stabilizes cathode surface, but also prevents electrolyte decomposition. Moreover, homogenously distributed B containing species serves as a skeleton to form more uniform and denser CEI, reducing the interphasial resistance. Remarkably, the Li/NMC811 cell with the TTFEB additive delivers an exceptional cycling stability with a high-capacity retention of 72.8% after 350 electrochemical cycles at a 1 C current rate, which is significantly higher than that of the cell cycled in the conventional electrolyte (59.7%). These findings provide a feasible pathway for improving the electrochemical performance of Ni-rich NMCs cathode by regulating the interphasial chemistry.
{"title":"Improved cyclic stability of LiNi0.8Mn0.1Co0.1O2 cathode enabled by a novel CEI forming additive","authors":"Zulipiya Shadike, Yiming Chen, Lin Liu, Xinyin Cai, Shuiyun Shen, Junliang Zhang","doi":"10.1007/s11708-024-0953-5","DOIUrl":"10.1007/s11708-024-0953-5","url":null,"abstract":"<div><p>The undesired side reactions at electrode/electrolyte interface as well as the irreversible phase evolution during electrochemical cycling significantly affect the cyclic performances of nickel-rich NMCs electrode materials. Electrolyte optimization is an effective approach to suppress such an adverse side reaction, thereby enhancing the electrochemical properties. Herein, a novel boron-based film forming additive, tris(2,2,2-trifluoroethyl) borate (TTFEB), has been introduced to regulate the interphasial chemistry of LiNi<sub>0.8</sub>Mn<sub>0.1</sub>Co<sub>0.1</sub>O<sub>2</sub> (NMC811) cathode to improve its long-term cyclability and rate properties. The results of multi-model diagnostic study reveal that formation lithium fluoride (LiF)-rich and boron (B) containing cathode electrolyte interphase (CEI) not only stabilizes cathode surface, but also prevents electrolyte decomposition. Moreover, homogenously distributed B containing species serves as a skeleton to form more uniform and denser CEI, reducing the interphasial resistance. Remarkably, the Li/NMC811 cell with the TTFEB additive delivers an exceptional cycling stability with a high-capacity retention of 72.8% after 350 electrochemical cycles at a 1 C current rate, which is significantly higher than that of the cell cycled in the conventional electrolyte (59.7%). These findings provide a feasible pathway for improving the electrochemical performance of Ni-rich NMCs cathode by regulating the interphasial chemistry.</p></div>","PeriodicalId":570,"journal":{"name":"Frontiers in Energy","volume":"18 4","pages":"535 - 544"},"PeriodicalIF":3.1,"publicationDate":"2024-07-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141745961","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-07-10DOI: 10.1007/s11708-024-0950-8
Jing Xue, Zhenlin Chen, Yuchao Zhang, Jincai Zhao
Utilizing plasmonic effects to assist electrochemical reactions exhibits a huge potential in tuning the reaction activities and product selectivity, which is most appealing especially in chemical reactions with multiple products, such as CO2 reduction reaction (CO2RR). However, a comprehensive review of the development and the underlying mechanisms in plasmon-assisted electrocatalytic CO2RR remains few and far between. Herein, the fundamentals of localized surface plasmonic resonance (LSPR) excitation and the properties of typical plasmonic metals (including Au, Ag, and Cu) are retrospected. Subsequently, the potential mechanisms of plasmonic effects (such as hot carrier effects and photothermal effects) on the reaction performance in the field of plasmon-assisted electrocatalytic CO2RR are summarized, which provides directions for the future development of this field. It is concluded that plasmonic catalysts exhibit potential capabilities in enhancing CO2RR while more in situ techniques are essential to further clarify the inner mechanisms.
{"title":"A review on plasmonic enhancement of activity and selectivity in electrocatalytic CO2 reduction","authors":"Jing Xue, Zhenlin Chen, Yuchao Zhang, Jincai Zhao","doi":"10.1007/s11708-024-0950-8","DOIUrl":"10.1007/s11708-024-0950-8","url":null,"abstract":"<div><p>Utilizing plasmonic effects to assist electrochemical reactions exhibits a huge potential in tuning the reaction activities and product selectivity, which is most appealing especially in chemical reactions with multiple products, such as CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR). However, a comprehensive review of the development and the underlying mechanisms in plasmon-assisted electrocatalytic CO2RR remains few and far between. Herein, the fundamentals of localized surface plasmonic resonance (LSPR) excitation and the properties of typical plasmonic metals (including Au, Ag, and Cu) are retrospected. Subsequently, the potential mechanisms of plasmonic effects (such as hot carrier effects and photothermal effects) on the reaction performance in the field of plasmon-assisted electrocatalytic CO<sub>2</sub>RR are summarized, which provides directions for the future development of this field. It is concluded that plasmonic catalysts exhibit potential capabilities in enhancing CO<sub>2</sub>RR while more <i>in situ</i> techniques are essential to further clarify the inner mechanisms.</p></div>","PeriodicalId":570,"journal":{"name":"Frontiers in Energy","volume":"18 4","pages":"399 - 417"},"PeriodicalIF":3.1,"publicationDate":"2024-07-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141835590","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-06-30DOI: 10.1007/s11708-024-0952-6
Juntian Niu, Shengzhuo Chen, Xianrong Zheng, Haiyu Liu, Yan Jin, Jingyu Ran
In recent years, the dry reforming of methane (DRM) reaction has gained widespread attention due to its effective utilization of two major greenhouse gases. Supported Ni-based catalysts for DRM exhibit a strong dependence on particle size, however, the reaction mechanisms involved remain unclear. In this work, the effect of metal particle size on CO2 activation and CO formation was explored in the DRM reaction using the density functional theory. Nix/MgO (x = 13, 25, 37) was constructed to investigate the CO2 activation and the formation of CO during the DRM reaction. It is found that CO2 is more inclined to undergo chemisorption on Nix/MgO before activation. With the variation in particle size, the main activation pathway of CO2 on the catalyst changes. On the smallest Ni13/MgO, CO2 tends to directly dissociate, while on the larger Ni25/MgO and Ni37/MgO, the hydrogenation dissociation of CO2 is more kinetically favorable. Compared to Ni13/MgO and Ni37/MgO, the oxidation of surface C atoms and the oxidation of CH occur more readily on Ni25/MgO. This indicates that C atoms are less likely to form on Ni25 particle and are more easily to be oxidized. To some extent, the results suggest that Ni25/MgO exhibits superior resistance to carbon formation.
近年来,甲烷干重整(DRM)反应因其对两种主要温室气体的有效利用而受到广泛关注。用于 DRM 的支撑镍基催化剂表现出与颗粒尺寸的强烈相关性,但其中涉及的反应机理仍不清楚。本研究利用密度泛函理论探讨了 DRM 反应中金属颗粒大小对 CO2 活化和 CO 生成的影响。构建了 Nix/MgO(x = 13、25、37)来研究 DRM 反应过程中 CO2 的活化和 CO 的形成。研究发现,二氧化碳在活化之前更倾向于在 Nix/MgO 上发生化学吸附。随着颗粒大小的变化,CO2 在催化剂上的主要活化途径也发生了变化。在最小的 Ni13/MgO 上,二氧化碳倾向于直接解离,而在较大的 Ni25/MgO 和 Ni37/MgO 上,二氧化碳的加氢解离在动力学上更为有利。与 Ni13/MgO 和 Ni37/MgO 相比,表面 C 原子的氧化和 CH 的氧化在 Ni25/MgO 上更容易发生。这表明 C 原子不太可能在 Ni25 颗粒上形成,而且更容易被氧化。在某种程度上,这些结果表明 Ni25/MgO 具有更强的抗碳形成能力。
{"title":"Impact of Ni particle size on CO2 activation and CO formation during reforming process: A density functional theory study","authors":"Juntian Niu, Shengzhuo Chen, Xianrong Zheng, Haiyu Liu, Yan Jin, Jingyu Ran","doi":"10.1007/s11708-024-0952-6","DOIUrl":"10.1007/s11708-024-0952-6","url":null,"abstract":"<div><p>In recent years, the dry reforming of methane (DRM) reaction has gained widespread attention due to its effective utilization of two major greenhouse gases. Supported Ni-based catalysts for DRM exhibit a strong dependence on particle size, however, the reaction mechanisms involved remain unclear. In this work, the effect of metal particle size on CO<sub>2</sub> activation and CO formation was explored in the DRM reaction using the density functional theory. Ni<i>x</i>/MgO (<i>x</i> = 13, 25, 37) was constructed to investigate the CO<sub>2</sub> activation and the formation of CO during the DRM reaction. It is found that CO<sub>2</sub> is more inclined to undergo chemisorption on Ni<i>x</i>/MgO before activation. With the variation in particle size, the main activation pathway of CO<sub>2</sub> on the catalyst changes. On the smallest Ni13/MgO, CO<sub>2</sub> tends to directly dissociate, while on the larger Ni25/MgO and Ni37/MgO, the hydrogenation dissociation of CO<sub>2</sub> is more kinetically favorable. Compared to Ni13/MgO and Ni37/MgO, the oxidation of surface C atoms and the oxidation of CH occur more readily on Ni25/MgO. This indicates that C atoms are less likely to form on Ni25 particle and are more easily to be oxidized. To some extent, the results suggest that Ni25/MgO exhibits superior resistance to carbon formation.</p></div>","PeriodicalId":570,"journal":{"name":"Frontiers in Energy","volume":"18 4","pages":"525 - 534"},"PeriodicalIF":3.1,"publicationDate":"2024-06-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141586159","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}