Pub Date : 2024-11-15DOI: 10.1016/j.ijhydene.2024.11.142
Jueshuo Fan , Lisha Shen , Chenglin Zhao , Zhida Wang , Zhiming Tu , Jiaxuan Hu , Changfeng Yan
Nickel selenide (NiSe) and carbon nanotubes (CNTs) heterojunction structure water electrolysis catalyst was prepared by vapor deposition method, constructing a heterogeneous phase interface between NiSe and CNTs. The interface effect between NiSe and CNTs enhanced further π-electron delocalization of CNTs, increasing the local electron density at the Ni sites. Subsequent ionic liquids (ILs) treatment further resolved the aggregation issues of NiSe nanoparticles and carbon nanotubes, and facilitated further π-electron delocalization at the heterojunction. The imidazolium cations acted as “connectors,” tightly linking the CNTs and NiSe nanoparticles. The NiSe/CNT-IL exhibited an HER overpotential of 82 mV at 10 mA cm⁻2 in 1 M KOH. Additionally, as a full water electrolysis catalyst in a water electrolyzer, it achieved a single-cell voltage of 1.965 V at a maximum current density of 500 mA cm⁻2 at 60 °C. This direct IL functionalization for CNTs facilitates the electron transfer process and ILs can serve as the electron acceptor with superior hydrogen adsorption.
利用气相沉积法制备了硒化镍（NiSe）和碳纳米管（CNTs）异质结结构水电解催化剂，在硒化镍和碳纳米管之间构建了异质相界面。NiSe 和 CNTs 之间的界面效应进一步增强了 CNTs 的 π 电子析出，提高了 Ni 位点的局部电子密度。随后的离子液体（ILs）处理进一步解决了硒化镍纳米粒子和碳纳米管的聚集问题，并促进了异质结处的π电子脱ocal。咪唑阳离子起着 "连接器 "的作用，将碳纳米管和 NiSe 纳米粒子紧密连接在一起。在 1 M KOH 中，当电流为 10 mA cm-2 时，NiSe/CNT-IL 的 HER 过电位为 82 mV。此外，作为水电解槽中的全水电解催化剂，它在 60 °C 条件下以 500 mA cm-2 的最大电流密度实现了 1.965 V 的单电池电压。这种对 CNTs 的直接 IL 功能化促进了电子转移过程，ILs 可作为电子受体，并具有优异的氢吸附性。
{"title":"Ion liquid treatment for high-performance NiSe/CNT water electrolysis catalyst","authors":"Jueshuo Fan , Lisha Shen , Chenglin Zhao , Zhida Wang , Zhiming Tu , Jiaxuan Hu , Changfeng Yan","doi":"10.1016/j.ijhydene.2024.11.142","DOIUrl":"10.1016/j.ijhydene.2024.11.142","url":null,"abstract":"<div><div>Nickel selenide (NiSe) and carbon nanotubes (CNTs) heterojunction structure water electrolysis catalyst was prepared by vapor deposition method, constructing a heterogeneous phase interface between NiSe and CNTs. The interface effect between NiSe and CNTs enhanced further π-electron delocalization of CNTs, increasing the local electron density at the Ni sites. Subsequent ionic liquids (ILs) treatment further resolved the aggregation issues of NiSe nanoparticles and carbon nanotubes, and facilitated further π-electron delocalization at the heterojunction. The imidazolium cations acted as “connectors,” tightly linking the CNTs and NiSe nanoparticles. The NiSe/CNT-IL exhibited an HER overpotential of 82 mV at 10 mA cm⁻<sup>2</sup> in 1 M KOH. Additionally, as a full water electrolysis catalyst in a water electrolyzer, it achieved a single-cell voltage of 1.965 V at a maximum current density of 500 mA cm⁻<sup>2</sup> at 60 °C. This direct IL functionalization for CNTs facilitates the electron transfer process and ILs can serve as the electron acceptor with superior hydrogen adsorption.</div></div>","PeriodicalId":337,"journal":{"name":"International Journal of Hydrogen Energy","volume":"94 ","pages":"Pages 774-781"},"PeriodicalIF":8.1,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142657251","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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 : 2024-11-15DOI: 10.1016/j.ijhydene.2024.11.056
Jiaming Lou , Yirui Lu , Daijun Yang , Xiangmin Pan , Bing Li , Pingwen Ming
The ionic conductivity of proton exchange membranes (PEMs) directly determines the ohmic resistance of proton exchange membrane fuel cells (PEMFCs), which is largely dependent on the membrane's hydration level. The structural differences between reinforced composite membranes (RCMs) and homogeneous membranes lead to distinct relationships between their hydration levels and ionic conductivity. In this study, Gore788.12 and Nafion®117 were selected as representatives of RCMs and homogeneous membranes, respectively. Experiments were designed to achieve operational conditions using a temperature and humidity chamber, wherein the PEM was weighed at equilibrium to calculate water uptake and water content, while EIS was employed to measure the membrane's ionic resistance and subsequently determine its conductivity, and HFR was utilized to compare the ohmic impedance of MEAs composed of two kinds of membrane under varying temperature and humidity conditions. In this study, the impacts of water activity on water uptake, water content, and ionic conductivity of the reinforced membrane are quantitatively analyzed. The results show that RCMs exhibit lower water content and ionic conductivity compared to homogeneous membranes, particularly at high water activity. The RCMs demonstrate lower ionic resistance and reduce dependence on water activity, resulting in lower ohmic resistance in MEAs using reinforced membranes. An empirical equation for ionic conductivity as a function of water activity is derived from experimental data. The semi-empirical equation between water content and water activity is modified based on the theoretical study of membrane water absorption mode under different water activity. This study can provide valuable insights for optimizing steady-state PEMFC simulation models.
质子交换膜（PEM）的离子导电率直接决定了质子交换膜燃料电池（PEMFC）的欧姆电阻，而欧姆电阻在很大程度上取决于膜的水合水平。增强复合膜（RCM）与均质膜之间的结构差异导致其水合水平与离子电导率之间的关系截然不同。本研究选择 Gore788.12 和 Nafion®117 分别作为 RCM 和均质膜的代表。实验设计使用温湿度室来实现操作条件，在平衡状态下称量 PEM，以计算吸水率和含水率；使用 EIS 测量膜的离子电阻，然后确定其电导率；使用 HFR 比较由两种膜组成的 MEA 在不同温湿度条件下的欧姆阻抗。本研究定量分析了水活性对增强膜的吸水率、含水率和离子电导率的影响。结果表明，与均质膜相比，RCM 的含水量和离子电导率较低，尤其是在高水活度条件下。RCM 具有较低的离子电阻，降低了对水活性的依赖性，从而降低了使用增强膜的 MEA 的欧姆电阻。根据实验数据得出了离子电导率与水活度函数的经验方程。根据对不同水活度下膜吸水模式的理论研究，修改了水含量与水活度之间的半经验方程。这项研究可为优化稳态 PEMFC 模拟模型提供有价值的见解。
{"title":"Experimental and model refinement of water content and membrane conductivity in reinforced composite proton exchange membranes","authors":"Jiaming Lou , Yirui Lu , Daijun Yang , Xiangmin Pan , Bing Li , Pingwen Ming","doi":"10.1016/j.ijhydene.2024.11.056","DOIUrl":"10.1016/j.ijhydene.2024.11.056","url":null,"abstract":"<div><div>The ionic conductivity of proton exchange membranes (PEMs) directly determines the ohmic resistance of proton exchange membrane fuel cells (PEMFCs), which is largely dependent on the membrane's hydration level. The structural differences between reinforced composite membranes (RCMs) and homogeneous membranes lead to distinct relationships between their hydration levels and ionic conductivity. In this study, Gore788.12 and Nafion®117 were selected as representatives of RCMs and homogeneous membranes, respectively. Experiments were designed to achieve operational conditions using a temperature and humidity chamber, wherein the PEM was weighed at equilibrium to calculate water uptake and water content, while EIS was employed to measure the membrane's ionic resistance and subsequently determine its conductivity, and HFR was utilized to compare the ohmic impedance of MEAs composed of two kinds of membrane under varying temperature and humidity conditions. In this study, the impacts of water activity on water uptake, water content, and ionic conductivity of the reinforced membrane are quantitatively analyzed. The results show that RCMs exhibit lower water content and ionic conductivity compared to homogeneous membranes, particularly at high water activity. The RCMs demonstrate lower ionic resistance and reduce dependence on water activity, resulting in lower ohmic resistance in MEAs using reinforced membranes. An empirical equation for ionic conductivity as a function of water activity is derived from experimental data. The semi-empirical equation between water content and water activity is modified based on the theoretical study of membrane water absorption mode under different water activity. This study can provide valuable insights for optimizing steady-state PEMFC simulation models.</div></div>","PeriodicalId":337,"journal":{"name":"International Journal of Hydrogen Energy","volume":"94 ","pages":"Pages 756-764"},"PeriodicalIF":8.1,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142657010","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
To develop non-noble electrocatalysts with high activity and stability for oxygen evolution reaction (OER)/urea oxidation reaction (UOR) is crucial to boost the efficiency of overall water/urea splitting reaction (OWS/OUS) for H2 production. Herein, we synthesized novel CeO2/Co(OH)2/FeS nanosheet arrays on nickel foam (CeO2/Co(OH)2/FeS@NF) through a simple two-step hydrothermal and following solvothermal routine. In this special structure, the ultra-thin 2D nanosheet morphology can adequately offer large contact area and thus abundant of active sites, facilitating significantly the mass transfer. Furthermore, the incorporation of FeS into CeO2/Co(OH)2 will not only modify the electron structure but also provide a number of phase interfaces, which can improve the inherent electron conductivity and promote the electron transport. More importantly, the rich oxygen vacancies (Ov) sites can vary the coordination of metal centers, modulating both the charge distribution and M−O bonding strength. As results, the CeO2/Co(OH)2/FeS@NF shows superior low overpotentials of 178 mV/1.30 V at 10 mA cm−2 to OER/UOR. The activity keeps its low value of 232 mV/1.375 V even when the current density was increased to as high as 300 mA cm−2. More importantly, the electrode of CeO2/Co(OH)2/FeS@NF//CeO2/Co(OH)2/FeS@NF just requires a low cell voltage of 1.41 V to realize OUS at a current density of 10 mA cm−2. Specifically, we also realized solar-driven H2 production. Plenty of H2 bubbles were continuously generated with a high speed of 600 L h−1 m−2 on the working electrode surface once the solar panel was placed under the natural sunlight.
开发具有高活性和稳定性的氧进化反应（OER）/尿素氧化反应（UOR）非贵金属电催化剂，对于提高整体水/尿素分离反应（OWS/OUS）生产 H2 的效率至关重要。在此，我们通过简单的两步水热法和溶热法在泡沫镍上合成了新型 CeO2/Co(OH)2/FeS 纳米片阵列（CeO2/Co(OH)2/FeS@NF）。在这种特殊的结构中，超薄的二维纳米片形态可以提供足够大的接触面积，从而提供丰富的活性位点，极大地促进了传质。此外，CeO2/Co(OH)2 中加入 FeS 不仅能改变电子结构，还能提供多个相界面，从而提高固有电子导电性，促进电子传输。更重要的是，丰富的氧空位（Ov）可改变金属中心的配位，调节电荷分布和 M-O 键强度。结果表明，CeO2/Co(OH)2/FeS@NF 与 OER/UOR 相比，在 10 mA cm-2 的过电位分别为 178 mV/1.30 V。即使电流密度增加到 300 mA cm-2 时，其活性仍保持在 232 mV/1.375 V 的低值。更重要的是，CeO2/Co(OH)2/FeS@NF//CeO2/Co(OH)2/FeS@NF 的电极只需要 1.41 V 的低电池电压，就能在 10 mA cm-2 的电流密度下实现 OUS。具体来说，我们还实现了太阳能驱动的 H2 生产。将太阳能电池板置于自然阳光下后，大量的 H2 气泡以 600 L h-1 m-2 的高速在工作电极表面不断生成。
{"title":"Construction of CeO2/Co(OH)2/FeS@NF nanosheet arrays for high-performance electrocatalytic oxygen evolution/urea oxidation, and overall water/urea splitting reactions","authors":"Fei Duan, Yunqin Hu, Junfeng Lin, Mingyue Li, Hao Wu, Zhiqing Cui, Caihong Fang","doi":"10.1016/j.ijhydene.2024.11.141","DOIUrl":"10.1016/j.ijhydene.2024.11.141","url":null,"abstract":"<div><div>To develop non-noble electrocatalysts with high activity and stability for oxygen evolution reaction (OER)/urea oxidation reaction (UOR) is crucial to boost the efficiency of overall water/urea splitting reaction (OWS/OUS) for H<sub>2</sub> production. Herein, we synthesized novel CeO<sub>2</sub>/Co(OH)<sub>2</sub>/FeS nanosheet arrays on nickel foam (CeO<sub>2</sub>/Co(OH)<sub>2</sub>/FeS@NF) through a simple two-step hydrothermal and following solvothermal routine. In this special structure, the ultra-thin 2D nanosheet morphology can adequately offer large contact area and thus abundant of active sites, facilitating significantly the mass transfer. Furthermore, the incorporation of FeS into CeO<sub>2</sub>/Co(OH)<sub>2</sub> will not only modify the electron structure but also provide a number of phase interfaces, which can improve the inherent electron conductivity and promote the electron transport. More importantly, the rich oxygen vacancies (O<sub>v</sub>) sites can vary the coordination of metal centers, modulating both the charge distribution and M−O bonding strength. As results, the CeO<sub>2</sub>/Co(OH)<sub>2</sub>/FeS@NF shows superior low overpotentials of 178 mV/1.30 V at 10 mA cm<sup>−2</sup> to OER/UOR. The activity keeps its low value of 232 mV/1.375 V even when the current density was increased to as high as 300 mA cm<sup>−2</sup>. More importantly, the electrode of CeO<sub>2</sub>/Co(OH)<sub>2</sub>/FeS@NF//CeO<sub>2</sub>/Co(OH)<sub>2</sub>/FeS@NF just requires a low cell voltage of 1.41 V to realize OUS at a current density of 10 mA cm<sup>−2</sup>. Specifically, we also realized solar-driven H<sub>2</sub> production. Plenty of H<sub>2</sub> bubbles were continuously generated with a high speed of 600 L h<sup>−1</sup> m<sup>−2</sup> on the working electrode surface once the solar panel was placed under the natural sunlight.</div></div>","PeriodicalId":337,"journal":{"name":"International Journal of Hydrogen Energy","volume":"94 ","pages":"Pages 706-715"},"PeriodicalIF":8.1,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142657250","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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 : 2024-11-14DOI: 10.1016/j.ijhydene.2024.10.426
Yongxin Lu , Guotian Yang , Xinli Li , Jianguo Liu , Tianye Yang , Jiarui Liu
The new energy hydrogen production system is subject to intermittent fluctuations, which compromise efficiency and equipment lifespan. This study proposes a new dynamic power allocation and control strategy for hybrid hydrogen production systems. By using the Whale Algorithm Optimized Variable Modal Decomposition (WOA-VMD), the fluctuating power of new energy is quantitatively decomposed and reconstructed. Based on a multi-objective optimization function, low-frequency variation components and high-frequency fluctuation components are accurately allocated between alkaline electrolyzers (ALK) and proton exchange membrane electrolyzers (PEM). The strategy effectively improves the source-load balancing capability, reducing the low-frequency fluctuation rate by 60% and reducing the high-frequency power amplitude by 70%, significantly reducing the operational demands on ALK electrolyzers, the capacity requirements of PEM electrolyzers, and the need for energy storage configuration, while also increasing hydrogen production efficiency by 7%. Compared to existing methods, the strategy has a transparent analysis process, strong interpretability, and good data reusability, making it valuable for engineering applications.
{"title":"Dynamic power allocation for the new energy hybrid hydrogen production system based on WOA-VMD: Improving fluctuation balance and optimizing control strategy","authors":"Yongxin Lu , Guotian Yang , Xinli Li , Jianguo Liu , Tianye Yang , Jiarui Liu","doi":"10.1016/j.ijhydene.2024.10.426","DOIUrl":"10.1016/j.ijhydene.2024.10.426","url":null,"abstract":"<div><div>The new energy hydrogen production system is subject to intermittent fluctuations, which compromise efficiency and equipment lifespan. This study proposes a new dynamic power allocation and control strategy for hybrid hydrogen production systems. By using the Whale Algorithm Optimized Variable Modal Decomposition (WOA-VMD), the fluctuating power of new energy is quantitatively decomposed and reconstructed. Based on a multi-objective optimization function, low-frequency variation components and high-frequency fluctuation components are accurately allocated between alkaline electrolyzers (ALK) and proton exchange membrane electrolyzers (PEM). The strategy effectively improves the source-load balancing capability, reducing the low-frequency fluctuation rate by 60% and reducing the high-frequency power amplitude by 70%, significantly reducing the operational demands on ALK electrolyzers, the capacity requirements of PEM electrolyzers, and the need for energy storage configuration, while also increasing hydrogen production efficiency by 7%. Compared to existing methods, the strategy has a transparent analysis process, strong interpretability, and good data reusability, making it valuable for engineering applications.</div></div>","PeriodicalId":337,"journal":{"name":"International Journal of Hydrogen Energy","volume":"94 ","pages":"Pages 580-599"},"PeriodicalIF":8.1,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142657130","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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 : 2024-11-14DOI: 10.1016/j.ijhydene.2024.11.071
Wei Liu , Yunkui Dong , Liangliang Jiang , Yuanlong Wei , Jifang Wan
In the peak-shaving process of underground salt cavern hydrogen storage, the surrounding rock experiences periodic stress and temperature variations over decades, leading to the induction of thermal stress that may compromise the safe operation of the storage during hydrogen injection and extraction. This study utilizes existing research on thermal stress associated with gas injection and extraction in salt caverns to establish boundary conditions for numerical simulations based on analytical solutions of gas temperature and pressure over time. It investigates the impact of injection-extraction cycles and rates on cavern stability, employing the tensile failure criterion as an evaluation metric. The findings reveal: 1. Tensile failure in the surrounding rock predominantly occurs during hydrogen extraction, with higher extraction rates and more frequent cycles exacerbating this failure. 2. During hydrogen extraction, tensile stress in the surrounding rock increases, causing failure near the interlayers of the cavern wall. Although tensile failure does not occur during hydrogen injection, stress concentration appears at the interface between rock salt and interlayers. 3. To mitigate tensile failure, it is recommended to increase the minimum internal pressure of hydrogen storage from 0.3 to 0.4 times the vertical stress at the cavern roof when designing for the maximum hydrogen extraction rate based on the minimum operating internal pressure of the cavern. By identifying critical factors influencing tensile failure, this study offers valuable insights for optimizing operational parameters of underground hydrogen storage, ensuring long-term stability and reliability in response to evolving energy storage demands.
{"title":"Studying injection-extraction induced thermal stress on hydrogen storage cavern in bedded salt rocks","authors":"Wei Liu , Yunkui Dong , Liangliang Jiang , Yuanlong Wei , Jifang Wan","doi":"10.1016/j.ijhydene.2024.11.071","DOIUrl":"10.1016/j.ijhydene.2024.11.071","url":null,"abstract":"<div><div>In the peak-shaving process of underground salt cavern hydrogen storage, the surrounding rock experiences periodic stress and temperature variations over decades, leading to the induction of thermal stress that may compromise the safe operation of the storage during hydrogen injection and extraction. This study utilizes existing research on thermal stress associated with gas injection and extraction in salt caverns to establish boundary conditions for numerical simulations based on analytical solutions of gas temperature and pressure over time. It investigates the impact of injection-extraction cycles and rates on cavern stability, employing the tensile failure criterion as an evaluation metric. The findings reveal: 1. Tensile failure in the surrounding rock predominantly occurs during hydrogen extraction, with higher extraction rates and more frequent cycles exacerbating this failure. 2. During hydrogen extraction, tensile stress in the surrounding rock increases, causing failure near the interlayers of the cavern wall. Although tensile failure does not occur during hydrogen injection, stress concentration appears at the interface between rock salt and interlayers. 3. To mitigate tensile failure, it is recommended to increase the minimum internal pressure of hydrogen storage from 0.3 to 0.4 times the vertical stress at the cavern roof when designing for the maximum hydrogen extraction rate based on the minimum operating internal pressure of the cavern. By identifying critical factors influencing tensile failure, this study offers valuable insights for optimizing operational parameters of underground hydrogen storage, ensuring long-term stability and reliability in response to evolving energy storage demands.</div></div>","PeriodicalId":337,"journal":{"name":"International Journal of Hydrogen Energy","volume":"94 ","pages":"Pages 626-638"},"PeriodicalIF":8.1,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142657345","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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 : 2024-11-14DOI: 10.1016/j.ijhydene.2024.10.404
Adam Zaidi , Christopher de Leeuwe , Yongliang Yan , Matteo Fella , Wenting Hu , Ian S. Metcalfe , Vincenzo Spallina
Lanthanum Strontium Ferrite (LSF), as an oxygen carrier, is used for chemical looping H2 production and CO2 utilization. In this work, the first attempt to upscale and understand the heat and mass transfer using 400 g of LSF pellets in a dynamically operated packed bed reactor is carried out.
Experiments were conducted at 650–820 °C and 1–5 barg, evaluating the pellets' reactor heat management, phase stability, and mechanical integrity over 70 h for the high-temperature redox cycling in chemical looping water-gas shift (CL-WGS) and chemical looping reverse water-gas shift (CL-RWGS) reactions.
Key results at the reactor scale indicate a maximum cyclic average H2O-to-H2 conversion of 31%, with a peak oxygen carrier capacity for CL-WGS of 0.38 mmol/gLSF. In the case of CL-RWGS, a peak CO2-to-CO conversion of 99.8% was achieved, with an oxygen carrier capacity of 0.57 mmol/gLSF.
Reactor heat management for exothermic and endothermic redox reactions showed the ability to maintain a high temperature profile where the heat front lagged the reaction front over a 15 cm reactive bed length. A maximum ΔT of 45 °C and 35 °C were observed during the oxidation of the LSF bed with H2O and CO2, respectively. In the case of air oxidation, a maximum ΔT of 120 °C indicates that the reaction is more exothermic and can be used to raise the temperature of the bed especially if heat is required to sustain the process.
No evidence of material performance degradation was recorded over 70 h of testing, maintaining the pellets' operational cyclability, phase stability, and mechanical integrity. The results demonstrate the robustness of the material, and they are encouraging versus the scalability of LSF for chemical looping applications, into H2 production and CO2 utilization processes.
{"title":"Experimental investigation of La0.6Sr0.4FeO3 -δ pellets as oxygen carriers for chemical-looping applications","authors":"Adam Zaidi , Christopher de Leeuwe , Yongliang Yan , Matteo Fella , Wenting Hu , Ian S. Metcalfe , Vincenzo Spallina","doi":"10.1016/j.ijhydene.2024.10.404","DOIUrl":"10.1016/j.ijhydene.2024.10.404","url":null,"abstract":"<div><div>Lanthanum Strontium Ferrite (LSF), as an oxygen carrier, is used for chemical looping H<sub>2</sub> production and CO<sub>2</sub> utilization. In this work, the first attempt to upscale and understand the heat and mass transfer using 400 g of LSF pellets in a dynamically operated packed bed reactor is carried out.</div><div>Experiments were conducted at 650–820 °C and 1–5 bar<sub>g</sub>, evaluating the pellets' reactor heat management, phase stability, and mechanical integrity over 70 h for the high-temperature redox cycling in chemical looping water-gas shift (CL-WGS) and chemical looping reverse water-gas shift (CL-RWGS) reactions.</div><div>Key results at the reactor scale indicate a maximum cyclic average H<sub>2</sub>O-to-H<sub>2</sub> conversion of 31%, with a peak oxygen carrier capacity for CL-WGS of 0.38 mmol/g<sub>LSF</sub>. In the case of CL-RWGS, a peak CO<sub>2</sub>-to-CO conversion of 99.8% was achieved, with an oxygen carrier capacity of 0.57 mmol/g<sub>LSF</sub>.</div><div>Reactor heat management for exothermic and endothermic redox reactions showed the ability to maintain a high temperature profile where the heat front lagged the reaction front over a 15 cm reactive bed length. A maximum ΔT of 45 °C and 35 °C were observed during the oxidation of the LSF bed with H<sub>2</sub>O and CO<sub>2</sub>, respectively. In the case of air oxidation, a maximum ΔT of 120 °C indicates that the reaction is more exothermic and can be used to raise the temperature of the bed especially if heat is required to sustain the process.</div><div>No evidence of material performance degradation was recorded over 70 h of testing, maintaining the pellets' operational cyclability, phase stability, and mechanical integrity. The results demonstrate the robustness of the material, and they are encouraging versus the scalability of LSF for chemical looping applications, into H<sub>2</sub> production and CO<sub>2</sub> utilization processes.</div></div>","PeriodicalId":337,"journal":{"name":"International Journal of Hydrogen Energy","volume":"94 ","pages":"Pages 535-544"},"PeriodicalIF":8.1,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142657259","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
High-entropy alloys (HEAs) have a great potential in hydrogen storage applications. Developing an alloy showing remarkable hydrogen sorption capacity, close to ambient temperature without activating is a significant challenge for solid-state hydrogen storage. The present investigation was conducted to develop HEAs to satisfy these requirements. Accordingly, four novel equiatomic TiVCrFeTa, TiVCrFeZr, TiVCrCoTa and TiVCrCoZr HEAs were designed, fabricated and characterized to address their capability for the hydrogen storage application. Alloy design was accomplished based on empirical relations and thermodynamic calculations in order to obtain a microstructure containing both BCC and Laves phases using elements with different affinity to hydrogen. The thermodynamic calculations through CALPHAD predicted the presence of BCC/B2 phase together with C14 and C15 Laves phases in all designed alloys which was in good agreement with experimental analyses. Studies on hydrogen storage properties revealed that all alloys, except for TiVCrFeZr, are able to absorb hydrogen at 294 K and 30 bar without any activation process at a short incubation time. The results revealed that after activation, TiVCrFeZr and TiVCrCoZr alloys containing high volume fraction of Laves phase (∼40%) displayed the highest absorption capacity, with 2.3 and 1.6 wt% of hydrogen, respectively, at 294 K and 30 bar. In addition, the PCT curves proposed formation of solid solution of hydrides in TiVCrFeTa and TiVCrCoTa alloys at room temperature, however, TiVCrFeZr and TiVCrCoZr alloys provide a plateau region illustrating typical transition during hydrogen absorption. This study is a step forward to understanding necessities for developing advanced materials for the hydrogen storage.
{"title":"Hydrogen storage in TiVCr(Fe,Co)(Zr,Ta) multi-phase high-entropy alloys","authors":"Farzaneh Zareipour , Hamed Shahmir , Yi Huang , Abhishek Kumar Patel , Erika Michela Dematteis , Marcello Baricco","doi":"10.1016/j.ijhydene.2024.11.109","DOIUrl":"10.1016/j.ijhydene.2024.11.109","url":null,"abstract":"<div><div>High-entropy alloys (HEAs) have a great potential in hydrogen storage applications. Developing an alloy showing remarkable hydrogen sorption capacity, close to ambient temperature without activating is a significant challenge for solid-state hydrogen storage. The present investigation was conducted to develop HEAs to satisfy these requirements. Accordingly, four novel equiatomic TiVCrFeTa, TiVCrFeZr, TiVCrCoTa and TiVCrCoZr HEAs were designed, fabricated and characterized to address their capability for the hydrogen storage application. Alloy design was accomplished based on empirical relations and thermodynamic calculations in order to obtain a microstructure containing both BCC and Laves phases using elements with different affinity to hydrogen. The thermodynamic calculations through CALPHAD predicted the presence of BCC/B2 phase together with C14 and C15 Laves phases in all designed alloys which was in good agreement with experimental analyses. Studies on hydrogen storage properties revealed that all alloys, except for TiVCrFeZr, are able to absorb hydrogen at 294 K and 30 bar without any activation process at a short incubation time. The results revealed that after activation, TiVCrFeZr and TiVCrCoZr alloys containing high volume fraction of Laves phase (∼40%) displayed the highest absorption capacity, with 2.3 and 1.6 wt% of hydrogen, respectively, at 294 K and 30 bar. In addition, the PCT curves proposed formation of solid solution of hydrides in TiVCrFeTa and TiVCrCoTa alloys at room temperature, however, TiVCrFeZr and TiVCrCoZr alloys provide a plateau region illustrating typical transition during hydrogen absorption. This study is a step forward to understanding necessities for developing advanced materials for the hydrogen storage.</div></div>","PeriodicalId":337,"journal":{"name":"International Journal of Hydrogen Energy","volume":"94 ","pages":"Pages 639-649"},"PeriodicalIF":8.1,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142657264","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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 : 2024-11-14DOI: 10.1016/j.ijhydene.2024.11.167
Yaqian Zhang , Wenqian Xie , Yidan Yin , Weiyi Zhang , Haihong Bao , Qinglan Hao , Jie Chang , Botao Teng
Electrocatalytic production of hydrogen peroxide (H2O2) by two electron water oxidation reaction (2e-WOR) is an environmental process with low cost and devoid of H2O2 storage and transportation. ZnO is one of the important promising 2e-WOR catalysts with relatively high activity and selectivity of H2O2. However, the active sites and the effects of oxygen defects of ZnO remain unknown, which hampers the further improvement in H2O2 formation. To explore the active sites and develop Zn-based catalysts with high performance, Ni, Cu and Co ions are chosen to form M0.1Zn0.9O (M = Ni, Cu and Co) catalysts. Combining the experimental results with density functional theory (DFT) calculations, the active site of 2e-WOR on Zn-based catalysts is first discovered to be the 3-coordinated surface Zn without surface oxygen defects since oxygen defects result in a strong interaction of ·OH with catalyst and then impede the 2e-WOR process. Catalysts with high activity and selectivity for 2e-WOR should have small nano-particle sizes without oxygen defects. Co0.1Zn0.9O is obtained with high activity (35.3 mmol min−1·gcat−1) and selectivity (82%) of H2O2 at 3.2 V vs RHE. This work provides valuable perspectives for designing and developing high-performing catalysts in 2e-WOR reaction.
{"title":"Greatly boosted H2O2 activity in two-electron water oxidation reaction on Zn-based catalysts by doping engineering","authors":"Yaqian Zhang , Wenqian Xie , Yidan Yin , Weiyi Zhang , Haihong Bao , Qinglan Hao , Jie Chang , Botao Teng","doi":"10.1016/j.ijhydene.2024.11.167","DOIUrl":"10.1016/j.ijhydene.2024.11.167","url":null,"abstract":"<div><div>Electrocatalytic production of hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) by two electron water oxidation reaction (2e-WOR) is an environmental process with low cost and devoid of H<sub>2</sub>O<sub>2</sub> storage and transportation. ZnO is one of the important promising 2e-WOR catalysts with relatively high activity and selectivity of H<sub>2</sub>O<sub>2</sub>. However, the active sites and the effects of oxygen defects of ZnO remain unknown, which hampers the further improvement in H<sub>2</sub>O<sub>2</sub> formation. To explore the active sites and develop Zn-based catalysts with high performance, Ni, Cu and Co ions are chosen to form M<sub>0.1</sub>Zn<sub>0.9</sub>O (M = Ni, Cu and Co) catalysts. Combining the experimental results with density functional theory (DFT) calculations, the active site of 2e-WOR on Zn-based catalysts is first discovered to be the 3-coordinated surface Zn without surface oxygen defects since oxygen defects result in a strong interaction of <strong>·</strong>OH with catalyst and then impede the 2e-WOR process. Catalysts with high activity and selectivity for 2e-WOR should have small nano-particle sizes without oxygen defects. Co<sub>0.1</sub>Zn<sub>0.9</sub>O is obtained with high activity (35.3 mmol min<sup>−1</sup><strong>·</strong>g<sub>cat</sub><sup>−1</sup>) and selectivity (82%) of H<sub>2</sub>O<sub>2</sub> at 3.2 V vs RHE. This work provides valuable perspectives for designing and developing high-performing catalysts in 2e-WOR reaction.</div></div>","PeriodicalId":337,"journal":{"name":"International Journal of Hydrogen Energy","volume":"94 ","pages":"Pages 600-607"},"PeriodicalIF":8.1,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142657108","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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 : 2024-11-14DOI: 10.1016/j.ijhydene.2024.11.061
Joel A. Gordon , Nazmiye Balta-Ozkan , Anwar Ul Haq , Seyed Ali Nabavi
As the global energy transition progresses, a range of drivers and barriers will continue to shape consumer attitudes and behavioural intentions towards emerging low-carbon technologies. The innovation-decision process for technologies composing the residential sector such as hydrogen-fuelled heating and cooking appliances is inherently governed by the complex interplay between perceptual, cognitive, and emotional factors. In response, this study responds to the call for an integrated research perspective to advance theoretical and empirical insights on consumer engagement in the domestic hydrogen transition. Drawing on online survey data collected in the United Kingdom, where a policy decision on ‘hydrogen homes’ is set for 2026, this study systematically explores whether an integrated modelling approach supports higher levels of explanatory and predictive power. Leveraging the foundations of the unified theory of domestic hydrogen acceptance, the analysis suggests that production perceptions, public trust, perceived relative advantage, safety perceptions, knowledge and awareness, and positive emotions will shape consumer support for hydrogen homes. Conversely, perceived disruptive impacts, perceived socio-economic costs, financial perceptions, and negative emotions may impede the domestic hydrogen transition. Consumer acceptance stands to significantly shape deployment prospects for hydrogen boilers and hobs, which are perceived to be somewhat advantageous to natural gas appliances from a technological and safety perspective. The study attests to the predictive benefits of adopting an integrated theoretical perspective when modelling the early stages of the innovation-decision process, while acknowledging opportunities for leveraging innovative research approaches in the future. As national hydrogen economies gain traction, adopting a neuroscience-based approach may help deepen scientific understanding regarding the neural, psychological, and emotional signatures shaping consumer perspectives towards hydrogen homes.
{"title":"Modelling the innovation-decision process for hydrogen homes: An integrated model of consumer acceptance and adoption intention","authors":"Joel A. Gordon , Nazmiye Balta-Ozkan , Anwar Ul Haq , Seyed Ali Nabavi","doi":"10.1016/j.ijhydene.2024.11.061","DOIUrl":"10.1016/j.ijhydene.2024.11.061","url":null,"abstract":"<div><div>As the global energy transition progresses, a range of drivers and barriers will continue to shape consumer attitudes and behavioural intentions towards emerging low-carbon technologies. The innovation-decision process for technologies composing the residential sector such as hydrogen-fuelled heating and cooking appliances is inherently governed by the complex interplay between perceptual, cognitive, and emotional factors. In response, this study responds to the call for an integrated research perspective to advance theoretical and empirical insights on consumer engagement in the domestic hydrogen transition. Drawing on online survey data collected in the United Kingdom, where a policy decision on ‘hydrogen homes’ is set for 2026, this study systematically explores whether an integrated modelling approach supports higher levels of explanatory and predictive power. Leveraging the foundations of the unified theory of domestic hydrogen acceptance, the analysis suggests that production perceptions, public trust, perceived relative advantage, safety perceptions, knowledge and awareness, and positive emotions will shape consumer support for hydrogen homes. Conversely, perceived disruptive impacts, perceived socio-economic costs, financial perceptions, and negative emotions may impede the domestic hydrogen transition. Consumer acceptance stands to significantly shape deployment prospects for hydrogen boilers and hobs, which are perceived to be somewhat advantageous to natural gas appliances from a technological and safety perspective. The study attests to the predictive benefits of adopting an integrated theoretical perspective when modelling the early stages of the innovation-decision process, while acknowledging opportunities for leveraging innovative research approaches in the future. As national hydrogen economies gain traction, adopting a neuroscience-based approach may help deepen scientific understanding regarding the neural, psychological, and emotional signatures shaping consumer perspectives towards hydrogen homes.</div></div>","PeriodicalId":337,"journal":{"name":"International Journal of Hydrogen Energy","volume":"94 ","pages":"Pages 554-579"},"PeriodicalIF":8.1,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142657027","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-14DOI: 10.1016/j.ijhydene.2024.11.002
De Hu , FangZhou Wu , Xiyu Chen , Feng Yu , Zijun Wang , Wei Wang
Reducing the overpotentials of HER and OER is an effective approach for decreasing the cost of hydrogen production. Electrolytic water catalysts with enhanced performance has been a significant research focus for utilizing hydrogen energy. In this work, the synergistic effect of organic polymer materials and inorganic materials was utilized to prepare a reticulated catalyst (NiZn/PPy) with a fibrous PPy substrate modified with bimetallic MOF spheres, which exhibits good HER and OER properties. Its special fiber mesh structure reduces catalyst agglomeration, which exposes more active sites for improving the stability of the catalyst over extended periods of time. Furthermore, the incorporation of PPy results in an increase in pyrrole-N, pyridine-N, and graphite-N structures, leading to a greater number of reactive active sites. The construction of bimetallic MOFs modulates the valence state of the active site, thereby accelerating electron transfer during the reaction. The synergistic interaction among the components resulted in an HER overpotential of only 76 mV at 10 mA cm−2 and an OER overpotential of only 373 mV at 100 mA cm−2 in a 1 M KOH solution, achieving a total dissolved water overpotential of 1.605 V.
降低 HER 和 OER 的过电位是降低制氢成本的有效方法。性能更强的电解水催化剂一直是利用氢能的研究重点。本研究利用有机聚合物材料和无机材料的协同效应，制备了一种网状催化剂（NiZn/PPy），其纤维状 PPy 基底由双金属 MOF 球修饰，具有良好的 HER 和 OER 性能。其特殊的纤维网状结构减少了催化剂的团聚，从而暴露出更多的活性位点，提高了催化剂的长期稳定性。此外，PPy 的加入增加了吡咯-N、吡啶-N 和石墨-N 结构，从而增加了反应活性位点的数量。双金属 MOF 的构建调节了活性位点的价态，从而加速了反应过程中的电子转移。由于各成分之间的协同作用，在 1 M KOH 溶液中，10 mA cm-2 的 HER 过电位仅为 76 mV，100 mA cm-2 的 OER 过电位仅为 373 mV，总溶解水过电位为 1.605 V。
{"title":"2D mesh PPy facilitates Ni-based MOF electron modulation and transfer for enhancing electrocatalytic total water dissociation","authors":"De Hu , FangZhou Wu , Xiyu Chen , Feng Yu , Zijun Wang , Wei Wang","doi":"10.1016/j.ijhydene.2024.11.002","DOIUrl":"10.1016/j.ijhydene.2024.11.002","url":null,"abstract":"<div><div>Reducing the overpotentials of HER and OER is an effective approach for decreasing the cost of hydrogen production. Electrolytic water catalysts with enhanced performance has been a significant research focus for utilizing hydrogen energy. In this work, the synergistic effect of organic polymer materials and inorganic materials was utilized to prepare a reticulated catalyst (NiZn/PPy) with a fibrous PPy substrate modified with bimetallic MOF spheres, which exhibits good HER and OER properties. Its special fiber mesh structure reduces catalyst agglomeration, which exposes more active sites for improving the stability of the catalyst over extended periods of time. Furthermore, the incorporation of PPy results in an increase in pyrrole-N, pyridine-N, and graphite-N structures, leading to a greater number of reactive active sites. The construction of bimetallic MOFs modulates the valence state of the active site, thereby accelerating electron transfer during the reaction. The synergistic interaction among the components resulted in an HER overpotential of only 76 mV at 10 mA cm<sup>−2</sup> and an OER overpotential of only 373 mV at 100 mA cm<sup>−2</sup> in a 1 M KOH solution, achieving a total dissolved water overpotential of 1.605 V.</div></div>","PeriodicalId":337,"journal":{"name":"International Journal of Hydrogen Energy","volume":"94 ","pages":"Pages 525-534"},"PeriodicalIF":8.1,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142657368","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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