Pub Date : 2025-04-23DOI: 10.1016/j.jpowsour.2025.237130
Siyuan Yang , Chuanwei Li , Qian Zhang , Lipan Xin , Linan Li , Shibin Wang , Qidi Zhou , Zhiyong Wang
Anode-free solid-state batteries (AFSSBs) enable higher energy density without the need for excess lithium compared to conventional all solid-state batteries. However, heterogeneous nucleation at the interface of the current collector (CC) and solid electrolyte (SE) is prone to inducing Li dendrites, which hinders AFSSBs development. Delamination of the CC–SE interface, which involves interfacial work of adhesion, is required during the nucleation process. Herein, a thermodynamic model of heterogeneous nucleation related to interfacial work of adhesion and a bulge model of Li nucleation are established and Li nucleation and plating experiments are performed to investigate the effect of the work of adhesion on Li nucleation behavior. The results demonstrate that increasing the work of adhesion of the CC–SE interface extends the nucleation time while increasing the Li radius and decreasing the number density of Li nuclei. Larger Li nuclei reduce the pressure within the CC, which diminishes the driving force (overpotential) of nucleation and likelihood of short-circuiting. The study findings suggest that stronger work of adhesion facilitates homogeneous Li nucleation, providing insight for optimizing the interface in AFSSBs.
与传统的全固态电池相比，无阳极固态电池（AFSSBs）无需过量锂即可实现更高的能量密度。然而，集流体（CC）和固体电解质（SE）界面上的异质成核容易诱发锂枝晶，从而阻碍无阳极固态电池的发展。在成核过程中需要对 CC-SE 界面进行分层，这涉及界面粘附功。本文建立了与界面附着功相关的异质成核热力学模型和锂成核凸起模型，并进行了锂成核和电镀实验，以研究附着功对锂成核行为的影响。结果表明，增加 CC-SE 界面的附着功可以延长成核时间，同时增加锂半径并降低锂核的数量密度。较大的锂核会降低 CC 内的压力，从而减小成核的驱动力（过电位）和短路的可能性。研究结果表明，更强的粘附功有利于均匀的锂核形成，为优化 AFSSB 的界面提供了启示。
{"title":"Li nucleation in anode-free solid-state Batteries: The role of interfacial mechanics","authors":"Siyuan Yang , Chuanwei Li , Qian Zhang , Lipan Xin , Linan Li , Shibin Wang , Qidi Zhou , Zhiyong Wang","doi":"10.1016/j.jpowsour.2025.237130","DOIUrl":"10.1016/j.jpowsour.2025.237130","url":null,"abstract":"<div><div>Anode-free solid-state batteries (AFSSBs) enable higher energy density without the need for excess lithium compared to conventional all solid-state batteries. However, heterogeneous nucleation at the interface of the current collector (CC) and solid electrolyte (SE) is prone to inducing Li dendrites, which hinders AFSSBs development. Delamination of the CC–SE interface, which involves interfacial work of adhesion, is required during the nucleation process. Herein, a thermodynamic model of heterogeneous nucleation related to interfacial work of adhesion and a bulge model of Li nucleation are established and Li nucleation and plating experiments are performed to investigate the effect of the work of adhesion on Li nucleation behavior. The results demonstrate that increasing the work of adhesion of the CC–SE interface extends the nucleation time while increasing the Li radius and decreasing the number density of Li nuclei. Larger Li nuclei reduce the pressure within the CC, which diminishes the driving force (overpotential) of nucleation and likelihood of short-circuiting. The study findings suggest that stronger work of adhesion facilitates homogeneous Li nucleation, providing insight for optimizing the interface in AFSSBs.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"644 ","pages":"Article 237130"},"PeriodicalIF":8.1,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143860122","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 : 2025-04-23DOI: 10.1016/j.jpowsour.2025.237124
Xiaopan Wu , Yixiang Ou , Yi Feng , Hui Chen , Haoqi Wang , Feiqiang Li , Zhiqiang Che , Yue Zhang , Pengan Zong , Li Hou , Wenping Yuan , Qili Jiang , Xiaoping Ouyang
Synergistic optimization of conductivity and corrosion resistance in metallic bipolar plates (BPs) is crucial for improving the performance, reliability, and longevity of proton exchange membrane fuel cell (PEMFC) systems. In this study, three hydrogen-free carbon-based nanocomposite coatings (Cr, Ti)/(Cr, Ti)-C-N/C were deposited on AISI austenitic stainless steel (SS316L) BPs using pulsed DC magnetron sputtering. The Ti/TiCN/C coatings demonstrate superior performance, characterized by smooth, uniform, and dense microstructure comprising Ti adhesion layer, TiCN transition layer and top C layer. The Ti/TiCN/C coatings demonstrate the highest hardness (21.36 GPa), the largest H/E∗ (0.072) and H3/E∗2 (0.084) ratios, maximum coating-substrate adhesion (20.3 mN), and excellent corrosion resistance in acidic conditions (pH = 3, H2SO4 + 0.1 ppm HF, 80 °C). Enhanced performances stem from the microstructural uniformity, strong interfacial bonding, and the regulating effect of the intermediate transition layer on the top C layer. Additionally, the Ti/TiCN/C coatings achieve the lowest interfacial contact resistance value of 2.4 mΩ·cm2, which is attributed to the maximum content and degree of disorder of C sp2, and the highest sp2/sp3 ratio in the top C layer. These results highlight Ti/TiCN/C coatings as a cost-effective, durable solution for high-performance PEMFC BPs, thereby offering a foundation for industrial-scale applications.
{"title":"The enhanced conductivity and corrosion resistance of hydrogen-free carbon-based nanocomposite coatings","authors":"Xiaopan Wu , Yixiang Ou , Yi Feng , Hui Chen , Haoqi Wang , Feiqiang Li , Zhiqiang Che , Yue Zhang , Pengan Zong , Li Hou , Wenping Yuan , Qili Jiang , Xiaoping Ouyang","doi":"10.1016/j.jpowsour.2025.237124","DOIUrl":"10.1016/j.jpowsour.2025.237124","url":null,"abstract":"<div><div>Synergistic optimization of conductivity and corrosion resistance in metallic bipolar plates (BPs) is crucial for improving the performance, reliability, and longevity of proton exchange membrane fuel cell (PEMFC) systems. In this study, three hydrogen-free carbon-based nanocomposite coatings (Cr, Ti)/(Cr, Ti)-C-N/C were deposited on AISI austenitic stainless steel (SS316L) BPs using pulsed DC magnetron sputtering. The Ti/TiCN/C coatings demonstrate superior performance, characterized by smooth, uniform, and dense microstructure comprising Ti adhesion layer, TiCN transition layer and top C layer. The Ti/TiCN/C coatings demonstrate the highest hardness (21.36 GPa), the largest H/E∗ (0.072) and H<sup>3</sup>/E∗<sup>2</sup> (0.084) ratios, maximum coating-substrate adhesion (20.3 mN), and excellent corrosion resistance in acidic conditions (pH = 3, H<sub>2</sub>SO<sub>4</sub> + 0.1 ppm HF, 80 °C). Enhanced performances stem from the microstructural uniformity, strong interfacial bonding, and the regulating effect of the intermediate transition layer on the top C layer. Additionally, the Ti/TiCN/C coatings achieve the lowest interfacial contact resistance value of 2.4 mΩ·cm<sup>2</sup>, which is attributed to the maximum content and degree of disorder of C sp<sup>2</sup>, and the highest sp<sup>2</sup>/sp<sup>3</sup> ratio in the top C layer. These results highlight Ti/TiCN/C coatings as a cost-effective, durable solution for high-performance PEMFC BPs, thereby offering a foundation for industrial-scale applications.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"644 ","pages":"Article 237124"},"PeriodicalIF":8.1,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143864486","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 : 2025-04-23DOI: 10.1016/j.jpowsour.2025.237048
Wei Han , Sihan Li , Jin Wang , Biao Shi , Qian Huang , Ying Zhao , Xiaodan Zhang
Perovskite/silicon tandem solar cells developed rapidly in recent years due to their high power conversion efficiency (PCE). However, minimizing the optical loss originated from reflection and parasitic absorption in transparent electrode is important to further improve the short circuit current density (JSC) of devices. Actually, zinc-doped indium oxide (IZO) and zirconium-doped indium oxide (IZrO) single layer thin films have certain shortcomings in terms of photoelectronic performance as transparent electrode in perovskite/silicon tandem solar cells. In this work, we designed and fabricated IZrO/IZO multilayer thin film that possesses improved electrical and optical properties compared to single layer films. The main reason comes from the IZrO/IZO multilayer thin film with better crystalline structure than that of single layer film. Additionally, the gradient refractive index in the IZrO/IZO multilayer thin film also plays a role in anti-reflection which promote the enhancement of JSC and then PCE. Finally, we obtained PCE of 30.74 % in the P-I-N type perovskite/silicon two-terminal tandem solar cell with an active area of 1.05 cm2 when applying IZrO/IZO multilayer thin film as the transparent electrode.
{"title":"IZrO/IZO multilayer thin film as transparent electrode in perovskite/silicon tandem solar cell","authors":"Wei Han , Sihan Li , Jin Wang , Biao Shi , Qian Huang , Ying Zhao , Xiaodan Zhang","doi":"10.1016/j.jpowsour.2025.237048","DOIUrl":"10.1016/j.jpowsour.2025.237048","url":null,"abstract":"<div><div>Perovskite/silicon tandem solar cells developed rapidly in recent years due to their high power conversion efficiency (PCE). However, minimizing the optical loss originated from reflection and parasitic absorption in transparent electrode is important to further improve the short circuit current density (<em>J</em><sub><em>SC</em></sub>) of devices. Actually, zinc-doped indium oxide (IZO) and zirconium-doped indium oxide (IZrO) single layer thin films have certain shortcomings in terms of photoelectronic performance as transparent electrode in perovskite/silicon tandem solar cells. In this work, we designed and fabricated IZrO/IZO multilayer thin film that possesses improved electrical and optical properties compared to single layer films. The main reason comes from the IZrO/IZO multilayer thin film with better crystalline structure than that of single layer film. Additionally, the gradient refractive index in the IZrO/IZO multilayer thin film also plays a role in anti-reflection which promote the enhancement of <em>J</em><sub><em>SC</em></sub> and then PCE. Finally, we obtained PCE of 30.74 % in the P-I-N type perovskite/silicon two-terminal tandem solar cell with an active area of 1.05 cm<sup>2</sup> when applying IZrO/IZO multilayer thin film as the transparent electrode.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"644 ","pages":"Article 237048"},"PeriodicalIF":8.1,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143864488","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}
This study explores the potential of sugarcane leaf-derived activated carbon (SLAC) as a novel support material for PtSnO2 electrocatalysts in direct ethanol fuel cell (DEFC). SLAC was synthesized via hydrothermal carbonization and activation processes to meet specific structural and surface requirements. Electrocatalysts were prepared using the polyol method and characterized through XRD, TEM, and XPS to analyze their physical and chemical properties. The investigation focused on the impact of carbon support impurities and the role of nitrogen doping on the electrochemical performance of ethanol oxidation reaction (EOR). The findings revealed that impurities in carbon support hindered performance by increasing onset potential and reducing current density due to blockage of the porous structure and disrupted electrostatic interactions between the bimetallic catalyst and the support. In contrast, N-doped SLAC improved performance by providing uniform metal dispersion, resulting in enhanced electron-rich sites. PtSnO2/N-doped SLAC exhibited superior performance, achieving the lowest onset potential, highest current density, and enhanced mass activity during EOR testing. This improvement is attributed to the synergistic effect of N-doped SLAC and SnO2, which provided electron-rich sites and improved CO tolerance through oxygen species that removed CO adsorption on the Pt surface. In DEFC testing, PtSnO2/N-doped SLAC demonstrated the highest performance, with an open circuit voltage (OCV) of 0.791 V, a peak current density of 350 mA/cm2, and a maximum power density of 65.07 mW/cm2. This work highlights the novel application of SLAC as a sustainable, high-performance support material for DEFC, offering insights into addressing impurity challenges and advancing clean energy technologies.
{"title":"Bimetallic nanocatalysts supported on sugarcane leaf-derived carbon for enhanced performance in direct alcohol fuel cells","authors":"Waritnan Wanchan , Rungsima Yeetsorn , Sanchai Kuboon , Anna Katharina Mechler , Piyush Kumar","doi":"10.1016/j.jpowsour.2025.237125","DOIUrl":"10.1016/j.jpowsour.2025.237125","url":null,"abstract":"<div><div>This study explores the potential of sugarcane leaf-derived activated carbon (SLAC) as a novel support material for PtSnO<sub>2</sub> electrocatalysts in direct ethanol fuel cell (DEFC). SLAC was synthesized via hydrothermal carbonization and activation processes to meet specific structural and surface requirements. Electrocatalysts were prepared using the polyol method and characterized through XRD, TEM, and XPS to analyze their physical and chemical properties. The investigation focused on the impact of carbon support impurities and the role of nitrogen doping on the electrochemical performance of ethanol oxidation reaction (EOR). The findings revealed that impurities in carbon support hindered performance by increasing onset potential and reducing current density due to blockage of the porous structure and disrupted electrostatic interactions between the bimetallic catalyst and the support. In contrast, N-doped SLAC improved performance by providing uniform metal dispersion, resulting in enhanced electron-rich sites. PtSnO<sub>2</sub>/N-doped SLAC exhibited superior performance, achieving the lowest onset potential, highest current density, and enhanced mass activity during EOR testing. This improvement is attributed to the synergistic effect of N-doped SLAC and SnO<sub>2</sub>, which provided electron-rich sites and improved CO tolerance through oxygen species that removed CO adsorption on the Pt surface. In DEFC testing, PtSnO<sub>2</sub>/N-doped SLAC demonstrated the highest performance, with an open circuit voltage (OCV) of 0.791 V, a peak current density of 350 mA/cm<sup>2</sup>, and a maximum power density of 65.07 mW/cm<sup>2</sup>. This work highlights the novel application of SLAC as a sustainable, high-performance support material for DEFC, offering insights into addressing impurity challenges and advancing clean energy technologies.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"644 ","pages":"Article 237125"},"PeriodicalIF":8.1,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143860125","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 : 2025-04-23DOI: 10.1016/j.jpowsour.2025.237119
Mehwish K. Butt , Fei Ye , Kong Long , Adel El-marghany , Yan Zhao , Javed Rehman , Zhi-Peng Li
A promising anode candidate with substantial potential is currently in high demand for alkali-ion batteries. In the current research, we studied the electronic and electrochemical properties of the newly reported carbon-rich C6BN monolayer as a potential anode material for Li/Na-ion batteries using density functional theory computation. Initial findings verify the structural, mechanical, thermal, dynamical and thermodynamic stability of the C6BN monolayer. As an anode material, the C6BN monolayer achieves a high theoretical Li/Na storage capacity (TSC) of 830/553 mA h g−1. The 2D C6BN surface exhibits a low diffusion barrier of 0.12 eV for Li and 0.09 eV for Na, enabling fast diffusion of Li/Na ions. The calculated average open circuit voltages (OCVs) of 0.47 V and 0.43 V for Li and Na adsorbed C6BN respectively, align well with commercial design requirements. Furthermore, an improved electrical conductivity in C6BN for Li/Na-ion batteries is noted. These remarkable findings position the 2D C6BN as a potential host material for Li/Na-ion batteries.
{"title":"Computational screening of C6BN monolayer as a promising anode material for Li/Na-ion batteries","authors":"Mehwish K. Butt , Fei Ye , Kong Long , Adel El-marghany , Yan Zhao , Javed Rehman , Zhi-Peng Li","doi":"10.1016/j.jpowsour.2025.237119","DOIUrl":"10.1016/j.jpowsour.2025.237119","url":null,"abstract":"<div><div>A promising anode candidate with substantial potential is currently in high demand for alkali-ion batteries. In the current research, we studied the electronic and electrochemical properties of the newly reported carbon-rich C<sub>6</sub>BN monolayer as a potential anode material for Li/Na-ion batteries using density functional theory computation. Initial findings verify the structural, mechanical, thermal, dynamical and thermodynamic stability of the C<sub>6</sub>BN monolayer. As an anode material, the C<sub>6</sub>BN monolayer achieves a high theoretical Li/Na storage capacity (TSC) of 830/553 mA h g<sup>−1</sup>. The 2D C<sub>6</sub>BN surface exhibits a low diffusion barrier of 0.12 eV for Li and 0.09 eV for Na, enabling fast diffusion of Li/Na ions. The calculated average open circuit voltages (OCVs) of 0.47 V and 0.43 V for Li and Na adsorbed C<sub>6</sub>BN respectively, align well with commercial design requirements. Furthermore, an improved electrical conductivity in C<sub>6</sub>BN for Li/Na-ion batteries is noted. These remarkable findings position the 2D C<sub>6</sub>BN as a potential host material for Li/Na-ion batteries.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"644 ","pages":"Article 237119"},"PeriodicalIF":8.1,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143860041","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 : 2025-04-23DOI: 10.1016/j.jpowsour.2025.237117
Xia Zhang , Yuqing Yang , Pengfei Jia , Shenao Li , Jishan Su , Shuwen Lv , Yizhan Sun , Ru Liu , Yuandong Xu , Wei Kong Pang
Cheese-like mangosteen shell derived activated carbon (MC) with high specific surface area and well-developed pore structure is prepared by one-step alkali activation method. Co3O4/MC composite is prepared by growing Co3O4 microspheres in MC pores via one-step hydrothermal method. Compared with individual Co3O4, Co3O4/MC composite exhibits excellent electrochemical property with the specific capacitance up to 324.4 F g−1. The MC skeleton has increased the physical strength of the composite and significantly reduced the charge transfer resistance of Co3O4. The asymmetric supercapacitor device Co3O4/MC//MC exhibits high specific capacitance of 80 F g−1 in the voltage window of 0∼1.6 V. Under the power density of 4000 W kg−1, the energy density can be as high as 27 Wh kg−1. After 10000 charge/discharge cycles, capacitance retention and coulombic efficiency are around 100%. The asymmetric supercapacitor device is used to light electronic meter and a red light-emitting diode, indicating the potential application in energy storage field.
一步碱活化法制备了具有高比表面积和发达孔隙结构的奶酪状山竹壳衍生活性炭（MC）。通过一步水热法在 MC 孔隙中生长 Co3O4 微球，制备出 Co3O4/MC 复合材料。与单个 Co3O4 相比，Co3O4/MC 复合材料具有优异的电化学性能，比电容高达 324.4 F g-1。MC 骨架提高了复合材料的物理强度，并显著降低了 Co3O4 的电荷转移电阻。不对称超级电容器装置 Co3O4/MC//MC 在 0∼1.6 V 的电压窗口内显示出 80 F g-1 的高比电容。在功率密度为 4000 W kg-1 的情况下，能量密度可高达 27 Wh kg-1。经过 10000 次充放电循环后，电容保持率和库仑效率约为 100%。该非对称超级电容器装置可用于点亮电子表和红色发光二极管，这表明它在储能领域具有潜在的应用前景。
{"title":"From biomass to energy storage materials: Mangosteen shells derived carbon doped Co3O4 as supercapacitor electrode materials","authors":"Xia Zhang , Yuqing Yang , Pengfei Jia , Shenao Li , Jishan Su , Shuwen Lv , Yizhan Sun , Ru Liu , Yuandong Xu , Wei Kong Pang","doi":"10.1016/j.jpowsour.2025.237117","DOIUrl":"10.1016/j.jpowsour.2025.237117","url":null,"abstract":"<div><div>Cheese-like mangosteen shell derived activated carbon (MC) with high specific surface area and well-developed pore structure is prepared by one-step alkali activation method. Co<sub>3</sub>O<sub>4</sub>/MC composite is prepared by growing Co<sub>3</sub>O<sub>4</sub> microspheres in MC pores via one-step hydrothermal method. Compared with individual Co<sub>3</sub>O<sub>4</sub>, Co<sub>3</sub>O<sub>4</sub>/MC composite exhibits excellent electrochemical property with the specific capacitance up to 324.4 F g<sup>−1</sup>. The MC skeleton has increased the physical strength of the composite and significantly reduced the charge transfer resistance of Co<sub>3</sub>O<sub>4</sub>. The asymmetric supercapacitor device Co<sub>3</sub>O<sub>4</sub>/MC//MC exhibits high specific capacitance of 80 F g<sup>−1</sup> in the voltage window of 0∼1.6 V. Under the power density of 4000 W kg<sup>−1</sup>, the energy density can be as high as 27 Wh kg<sup>−1</sup>. After 10000 charge/discharge cycles, capacitance retention and coulombic efficiency are around 100%. The asymmetric supercapacitor device is used to light electronic meter and a red light-emitting diode, indicating the potential application in energy storage field.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"644 ","pages":"Article 237117"},"PeriodicalIF":8.1,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143860225","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 : 2025-04-23DOI: 10.1016/j.jpowsour.2025.237126
Anyang Wang , Xiting Wang , Xuhao Wan , Jun Jia , Zeyuan Li , Xue Ke , Rong Han , Zhaofu Zhang , Jun Wang , Yuzheng Guo
Developing highly efficient oxygen electrocatalysts is crucial in solving environmental and energy challenges. Herein, we leverage the design flexibility of 2D conductive metal-organic frameworks (c-MOFs) to conduct a comprehensive investigation of the activity of transition metal-hexaminobenzene (TM-HAB) for oxygen evolution reaction/oxygen reduction reaction/hydrogen evolution reaction (OER/ORR/HER) based on density functional theory (DFT) calculations. TM-HABs show sufficient structural stability and feasible synthesis according to the formation energy and dissolution potential criteria. Remarkably, Co-HAB exhibits low overpotentials of 0.32 and 0.48 V for OER and ORR, while Rh-HAB displays low overpotentials of 0.02 and 0.38 V for HER and OER, suggesting that they hold great potential as bifunctional catalysts for rechargeable metal-air batteries and water splitting, respectively. Additional volcano and contour plots reveal activity trends. The origin of activity is investigated through the d-band center of TM and bonding analysis. Intrinsic descriptors requiring no DFT data are proposed for rapid prediction of catalytic activity. The role of oxide formation enthalpies for metal atoms in activity prediction is highlighted. Our study not only demonstrates the superior properties of conductive metal-organic frameworks as bifunctional electrocatalysts but also provides valuable insights for the design and discovery of efficient catalysts.
{"title":"Hexaminobenzene in conductive metal-organic frameworks as bifunctional electrocatalysts for overall water splitting and metal-air batteries","authors":"Anyang Wang , Xiting Wang , Xuhao Wan , Jun Jia , Zeyuan Li , Xue Ke , Rong Han , Zhaofu Zhang , Jun Wang , Yuzheng Guo","doi":"10.1016/j.jpowsour.2025.237126","DOIUrl":"10.1016/j.jpowsour.2025.237126","url":null,"abstract":"<div><div>Developing highly efficient oxygen electrocatalysts is crucial in solving environmental and energy challenges. Herein, we leverage the design flexibility of 2D conductive metal-organic frameworks (c-MOFs) to conduct a comprehensive investigation of the activity of transition metal-hexaminobenzene (TM-HAB) for oxygen evolution reaction/oxygen reduction reaction/hydrogen evolution reaction (OER/ORR/HER) based on density functional theory (DFT) calculations. TM-HABs show sufficient structural stability and feasible synthesis according to the formation energy and dissolution potential criteria. Remarkably, Co-HAB exhibits low overpotentials of 0.32 and 0.48 V for OER and ORR, while Rh-HAB displays low overpotentials of 0.02 and 0.38 V for HER and OER, suggesting that they hold great potential as bifunctional catalysts for rechargeable metal-air batteries and water splitting, respectively. Additional volcano and contour plots reveal activity trends. The origin of activity is investigated through the d-band center of TM and bonding analysis. Intrinsic descriptors requiring no DFT data are proposed for rapid prediction of catalytic activity. The role of oxide formation enthalpies for metal atoms in activity prediction is highlighted. Our study not only demonstrates the superior properties of conductive metal-organic frameworks as bifunctional electrocatalysts but also provides valuable insights for the design and discovery of efficient catalysts.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"644 ","pages":"Article 237126"},"PeriodicalIF":8.1,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143860126","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 : 2025-04-23DOI: 10.1016/j.jpowsour.2025.237100
Ming-Dai Yang , Sheng-Qiao Hu , Chang-Ping Li , Yein Kwak , Tae Jo Ko
To enhance the modeling accuracy of the two-dimensional lithium battery model and improve its precision in predicting the discharge process, this study proposes an approach based on a new discharge boundary condition setting. In this method, when a battery is connected to a load circuit, electrochemical reactions occurring at the interface between the electrode particles and the electrolyte induce uniform changes in the surface potentials of all electrode particles in the cathode and anode regions, rather than being confined to the battery terminals near the current collectors. These changes are quantified based on the load current using an optimization algorithm, instead of conductivity calculations. Leveraging this approach, a two-dimensional battery model is developed within an improved lattice Boltzmann method framework. Simulation results reveal that the model satisfies current and charge conservation principles, substantially improves computational accuracy, and demonstrates high stability. Furthermore, the two-dimensional local variations in lithium/lithium-ion concentrations predicted by the model align well with the general mechanism analysis. Notably, this model demonstrates versatility for broad applications, effectively predicting battery behavior under varied discharge conditions, such as constant-current and constant-resistance discharge modes, and can handle electrode particle size heterogeneity.
{"title":"Enhancing precision in two-dimensional lithium battery modeling using an improved discharge boundary condition setting within the lattice Boltzmann method framework for broad applications","authors":"Ming-Dai Yang , Sheng-Qiao Hu , Chang-Ping Li , Yein Kwak , Tae Jo Ko","doi":"10.1016/j.jpowsour.2025.237100","DOIUrl":"10.1016/j.jpowsour.2025.237100","url":null,"abstract":"<div><div>To enhance the modeling accuracy of the two-dimensional lithium battery model and improve its precision in predicting the discharge process, this study proposes an approach based on a new discharge boundary condition setting. In this method, when a battery is connected to a load circuit, electrochemical reactions occurring at the interface between the electrode particles and the electrolyte induce uniform changes in the surface potentials of all electrode particles in the cathode and anode regions, rather than being confined to the battery terminals near the current collectors. These changes are quantified based on the load current using an optimization algorithm, instead of conductivity calculations. Leveraging this approach, a two-dimensional battery model is developed within an improved lattice Boltzmann method framework. Simulation results reveal that the model satisfies current and charge conservation principles, substantially improves computational accuracy, and demonstrates high stability. Furthermore, the two-dimensional local variations in lithium/lithium-ion concentrations predicted by the model align well with the general mechanism analysis. Notably, this model demonstrates versatility for broad applications, effectively predicting battery behavior under varied discharge conditions, such as constant-current and constant-resistance discharge modes, and can handle electrode particle size heterogeneity.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"644 ","pages":"Article 237100"},"PeriodicalIF":8.1,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143860133","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 : 2025-04-23DOI: 10.1016/j.jpowsour.2025.237082
Jian-Ni Liu , Jian-Hua Cao , Yue-Yang Wu , Jia-Rui Zheng , Wei-Hua Liang , Da-Yong Wu
The safety concerns pose significant challenges to the development of a new generation of high-energy-density lithium-ion batteries. To avoid short circuiting, it is important to ensure that the separator does not shrink in case of battery overheating. We have developed a process for manufacturing composite membranes by dip-coating polyimide (PI) with polyethylene terephthalate (PET) non-woven fabric as the base film for future continuous mass production. This processing technique, vapor-induced and immersion precipitation phase separation to modulate the pore structure of the PI layer, obtained a PI-PET composite membrane with a porosity of 58 %, a pore size distribution between 25 and 90 nm, and an average pore size of about 65 nm. Additionally, the composite membrane exhibits excellent thermal stability, with a Td5 of 420 °C and no shrinkage after being heated at 250 °C for 1 h. The capacity retention of a LiNi0.5Co0.2Mn0.3O2|| graphite (NCM523||C) pouch battery assembled with the PI composite membrane is 60.4 % after 1000 cycles at 1C, comparable to the performance of pouch battery with the commercial Al2O3/PE/Al2O3 separator. In addition, the pouch battery assembled with the PI composite membrane passes destructive tests such as folding, needling, etc., and it continues to discharge for approximately 10 h after the corners are cut, demonstrating excellent safety features.
{"title":"Micro porous forming of polyimide composite membrane with temperature and humidity control and its application Evaluation in lithium-ion batteries","authors":"Jian-Ni Liu , Jian-Hua Cao , Yue-Yang Wu , Jia-Rui Zheng , Wei-Hua Liang , Da-Yong Wu","doi":"10.1016/j.jpowsour.2025.237082","DOIUrl":"10.1016/j.jpowsour.2025.237082","url":null,"abstract":"<div><div>The safety concerns pose significant challenges to the development of a new generation of high-energy-density lithium-ion batteries. To avoid short circuiting, it is important to ensure that the separator does not shrink in case of battery overheating. We have developed a process for manufacturing composite membranes by dip-coating polyimide (PI) with polyethylene terephthalate (PET) non-woven fabric as the base film for future continuous mass production. This processing technique, vapor-induced and immersion precipitation phase separation to modulate the pore structure of the PI layer, obtained a PI-PET composite membrane with a porosity of 58 %, a pore size distribution between 25 and 90 nm, and an average pore size of about 65 nm. Additionally, the composite membrane exhibits excellent thermal stability, with a T<sub>d5</sub> of 420 °C and no shrinkage after being heated at 250 °C for 1 h. The capacity retention of a LiNi<sub>0.5</sub>Co<sub>0.2</sub>Mn<sub>0.3</sub>O<sub>2</sub>|| graphite (NCM523||C) pouch battery assembled with the PI composite membrane is 60.4 % after 1000 cycles at 1C, comparable to the performance of pouch battery with the commercial Al<sub>2</sub>O<sub>3</sub>/PE/Al<sub>2</sub>O<sub>3</sub> separator. In addition, the pouch battery assembled with the PI composite membrane passes destructive tests such as folding, needling, etc., and it continues to discharge for approximately 10 h after the corners are cut, demonstrating excellent safety features.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"644 ","pages":"Article 237082"},"PeriodicalIF":8.1,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143860226","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 : 2025-04-23DOI: 10.1016/j.jpowsour.2025.237116
Axel Briand , Stefan Henfling , Marie Lamard , Sébastien Rosini , Bruno Auvity
This study examines the impact of chloride contamination on proton exchange membrane fuel cells (PEMFCs) in a marine environment, focusing on the physical state of NaCl contaminants. Results indicate that chloride diffusion through the membrane electrode assembly (MEA) is significantly slower when NaCl is in crystalline form compared to its dissolved state in water droplets. Chloride contamination in the aqueous phase leads to performance losses at lower concentrations, whereas solid-phase contamination requires much higher exposure levels for similar effects. Additionally, the gas diffusion layer (GDL) plays a key role in limiting the transport of solid NaCl particles. Despite these differences, the study concludes that under typical marine conditions, chloride containing contaminants do not induce substantial irreversible performance degradation. These findings provide new insights into PEMFC durability in maritime applications, emphasizing the importance of contaminant phase and environmental conditions.
{"title":"An attempt to assess the criticality of chlorides for PEMFC durability in a marine environment","authors":"Axel Briand , Stefan Henfling , Marie Lamard , Sébastien Rosini , Bruno Auvity","doi":"10.1016/j.jpowsour.2025.237116","DOIUrl":"10.1016/j.jpowsour.2025.237116","url":null,"abstract":"<div><div>This study examines the impact of chloride contamination on proton exchange membrane fuel cells (PEMFCs) in a marine environment, focusing on the physical state of NaCl contaminants. Results indicate that chloride diffusion through the membrane electrode assembly (MEA) is significantly slower when NaCl is in crystalline form compared to its dissolved state in water droplets. Chloride contamination in the aqueous phase leads to performance losses at lower concentrations, whereas solid-phase contamination requires much higher exposure levels for similar effects. Additionally, the gas diffusion layer (GDL) plays a key role in limiting the transport of solid NaCl particles. Despite these differences, the study concludes that under typical marine conditions, chloride containing contaminants do not induce substantial irreversible performance degradation. These findings provide new insights into PEMFC durability in maritime applications, emphasizing the importance of contaminant phase and environmental conditions.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"644 ","pages":"Article 237116"},"PeriodicalIF":8.1,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143864485","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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