Meiting Guo, Zhishan Li, Lang Tang, Jingwei Li, Zehua Wang, Bo Wang, Zongping Shao, San Ping Jiang, Zhongwei Yue
Due to the low activation energy and high mobility of proton transfer, protonic ceramic cells (PCCs), including protonic ceramic fuel cells (PCFCs) and protonic ceramic electrolysis cells (PCECs), working at relatively low temperatures (400-700 oC) gain increasing attention as promising and highly efficient energy conversion and storage technologies to replace the oxide ions conducting high temperature solid oxide cells (SOCs). Similar to SOCs, Fe-Cr based alloys are also commonly used as metallic interconnect in PCC stacks. However, the practical applicability of Ba-containing proton conducting electrolytes in PCCs is fundamentally related to their tolerance and resistance towards the deposition and poisoning of volatile chromium species from Fe-Cr based interconnect. This study focuses on the interaction between Cr species and most widely used proton conducting electrolyte, BaZr0.1Ce0.7Y0.1Yb0.1O3-δ (BZCYYb1711) within a temperature range from 400 ℃ to 700 ℃. The results indicate that barium oxide and BZCYYb1711 powder react with Cr2O3 powder at 250 ℃ and 400 ℃ respectively, while deposition of Cr species on the BZCYYb1711 electrolyte surface occurs at temperatures as low as 500 ℃. Ba segregates from BZCYYb1711 electrolytes and reacts with gaseous Cr species, forming BaCrO4 and causing the significant depreciation of Ba content in the electrolyte. Cr species also diffuse into the inner layer of BZCYYb1711, leading to the segregation of CeO2 and degrading the conductivity of the electrolyte. This study demonstrates the deposition and poisoning of Cr species from Fe-Cr based metallic interconnect is a serious issue for the practical and long-term applicability of Ba-containing protonic ceramic materials in PCCs.
{"title":"Chromium Deposition and Poisoning of Proton Conducting BaZr0.1Ce0.7Y0.1Yb0.1O3-δ Electrolyte of Protonic Ceramic Cells","authors":"Meiting Guo, Zhishan Li, Lang Tang, Jingwei Li, Zehua Wang, Bo Wang, Zongping Shao, San Ping Jiang, Zhongwei Yue","doi":"10.1039/d5ta01090j","DOIUrl":"https://doi.org/10.1039/d5ta01090j","url":null,"abstract":"Due to the low activation energy and high mobility of proton transfer, protonic ceramic cells (PCCs), including protonic ceramic fuel cells (PCFCs) and protonic ceramic electrolysis cells (PCECs), working at relatively low temperatures (400-700 oC) gain increasing attention as promising and highly efficient energy conversion and storage technologies to replace the oxide ions conducting high temperature solid oxide cells (SOCs). Similar to SOCs, Fe-Cr based alloys are also commonly used as metallic interconnect in PCC stacks. However, the practical applicability of Ba-containing proton conducting electrolytes in PCCs is fundamentally related to their tolerance and resistance towards the deposition and poisoning of volatile chromium species from Fe-Cr based interconnect. This study focuses on the interaction between Cr species and most widely used proton conducting electrolyte, BaZr0.1Ce0.7Y0.1Yb0.1O3-δ (BZCYYb1711) within a temperature range from 400 ℃ to 700 ℃. The results indicate that barium oxide and BZCYYb1711 powder react with Cr2O3 powder at 250 ℃ and 400 ℃ respectively, while deposition of Cr species on the BZCYYb1711 electrolyte surface occurs at temperatures as low as 500 ℃. Ba segregates from BZCYYb1711 electrolytes and reacts with gaseous Cr species, forming BaCrO4 and causing the significant depreciation of Ba content in the electrolyte. Cr species also diffuse into the inner layer of BZCYYb1711, leading to the segregation of CeO2 and degrading the conductivity of the electrolyte. This study demonstrates the deposition and poisoning of Cr species from Fe-Cr based metallic interconnect is a serious issue for the practical and long-term applicability of Ba-containing protonic ceramic materials in PCCs.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"1 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143832344","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Transition metal hydroxides have attracted significant interest as electrode materials for supercapacitors due to their abundant redox activity and excellent electrical conductivity. Here, we present the novel design and construction of a hexagonal thin nanosheet engineering of cobalt hydroxide (Co(OH)2) with enveloped imidazolium-based poly(ionic liquid)s (PIL-Br, poly(1-butyl-3-vinylimidazolium bromide). With the presence of PILs in the Co(OH)2 influences a morphogenesis control and high capacitance of 1758 F g-1 at 2 A g-1 current density in a three-electrode system. In-depth, a solid-state free-standing device has been developed with a unique electrolyte configuration comprising EMIM-TFSI/PVDF-HFP further enhances the device's performance. Achieving an high energy density of 212 Wh kg-1 at a power density of 1499 W kg-1 underscores its capability to deliver stored energy effectively. Most notably, the device demonstrates exceptional durability, maintaining a capacity retention of 97% even after undergoing 10,000 cycles at 5 A g-1. Density functional theory also indicates the presence of PILs active sites in the composites promising new in-situ strategy for energy storage applications.
{"title":"Architecture of imidazolium-based poly(ionic liquid)s-cobalt hexagonal thin nanosheet for high energy density with membrane electrolytes","authors":"Abhishek Narayanan, T. Pavan, Narad Barman, Nagaraj Naik, Ranjit Thapa, Chandra Sekhar Rout, Mahesh Padaki","doi":"10.1039/d4ta06914e","DOIUrl":"https://doi.org/10.1039/d4ta06914e","url":null,"abstract":"Transition metal hydroxides have attracted significant interest as electrode materials for supercapacitors due to their abundant redox activity and excellent electrical conductivity. Here, we present the novel design and construction of a hexagonal thin nanosheet engineering of cobalt hydroxide (Co(OH)2) with enveloped imidazolium-based poly(ionic liquid)s (PIL-Br, poly(1-butyl-3-vinylimidazolium bromide). With the presence of PILs in the Co(OH)2 influences a morphogenesis control and high capacitance of 1758 F g-1 at 2 A g-1 current density in a three-electrode system. In-depth, a solid-state free-standing device has been developed with a unique electrolyte configuration comprising EMIM-TFSI/PVDF-HFP further enhances the device's performance. Achieving an high energy density of 212 Wh kg-1 at a power density of 1499 W kg-1 underscores its capability to deliver stored energy effectively. Most notably, the device demonstrates exceptional durability, maintaining a capacity retention of 97% even after undergoing 10,000 cycles at 5 A g-1. Density functional theory also indicates the presence of PILs active sites in the composites promising new in-situ strategy for energy storage applications.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"40 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143832342","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Ademola Adeniji, Adrian Beda, Philippe Fioux, Camelia Matei Ghimbeu
Sodium-ion capacitors are increasingly gaining momentum thanks to their high energy and power densities. However, there is still a lack of understanding of porous carbon positive electrode properties that affect their electrochemical performance. To address this challenge, carbon materials with controlled porosity, structure and surface functionalities are strongly required. Herein, we report the synthesis of nitrogen-doped porous carbons (NDPCs) by a combined soft-salt templating approach, that allows to achieve various nitrogen doping levels (up to 8 at%) via precursor amount modification. This results in materials with ultrahigh specific surface area (up to 2412 m2 g−1) and finely tuned pore size (up to 0.92 nm) matching the desolvated PF6− anion sorption requirement of 0.8 nm, along with controlled graphitization induced by the salt type. The materials exhibit specific capacities ranging from 83 to 159 mA h g−1vs. Na/Na+, higher than that of commercial carbons. From positive linear correlations, it was identified that the improved capacity is driven by the large specific surface area, substantial microporous volume with appropriate pore size, and structural defects, which enhance ion adsorption and promote enhanced specific capacity. However, the capacity retention is improved by the mesoporous volume and graphitic domains. Moreover, the surface pseudocapacitive interactions involving Na+ and PF6− ions could be associated with specific oxygen-containing groups (phenol/ethers and anhydride) and nitrogen species (pyridinic-N/pyrrolic-N). The dual carbon full-cell configuration consisting of a hard carbon and N-doped carbon achieves a high energy density of 209 W h kg−1 and a maximum power density of 5040 W kg−1 with ∼100% coulombic efficiency.
{"title":"Engineering nitrogen-doped porous carbon positive electrodes for high-performance sodium-ion capacitors: the critical role of porosity, structure and surface functionalities","authors":"Ademola Adeniji, Adrian Beda, Philippe Fioux, Camelia Matei Ghimbeu","doi":"10.1039/d5ta01075f","DOIUrl":"https://doi.org/10.1039/d5ta01075f","url":null,"abstract":"Sodium-ion capacitors are increasingly gaining momentum thanks to their high energy and power densities. However, there is still a lack of understanding of porous carbon positive electrode properties that affect their electrochemical performance. To address this challenge, carbon materials with controlled porosity, structure and surface functionalities are strongly required. Herein, we report the synthesis of nitrogen-doped porous carbons (NDPCs) by a combined soft-salt templating approach, that allows to achieve various nitrogen doping levels (up to 8 at%) <em>via</em> precursor amount modification. This results in materials with ultrahigh specific surface area (up to 2412 m<small><sup>2</sup></small> g<small><sup>−1</sup></small>) and finely tuned pore size (up to 0.92 nm) matching the desolvated PF<small><sub>6</sub></small><small><sup>−</sup></small> anion sorption requirement of 0.8 nm, along with controlled graphitization induced by the salt type. The materials exhibit specific capacities ranging from 83 to 159 mA h g<small><sup>−1</sup></small> <em>vs.</em> Na/Na<small><sup>+</sup></small>, higher than that of commercial carbons. From positive linear correlations, it was identified that the improved capacity is driven by the large specific surface area, substantial microporous volume with appropriate pore size, and structural defects, which enhance ion adsorption and promote enhanced specific capacity. However, the capacity retention is improved by the mesoporous volume and graphitic domains. Moreover, the surface pseudocapacitive interactions involving Na<small><sup>+</sup></small> and PF<small><sub>6</sub></small><small><sup>−</sup></small> ions could be associated with specific oxygen-containing groups (phenol/ethers and anhydride) and nitrogen species (pyridinic-N/pyrrolic-N). The dual carbon full-cell configuration consisting of a hard carbon and N-doped carbon achieves a high energy density of 209 W h kg<small><sup>−1</sup></small> and a maximum power density of 5040 W kg<small><sup>−1</sup></small> with ∼100% coulombic efficiency.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"67 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143832120","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yulong He, Zicheng Luo, Hongfei Xu, Zehong Yuan, Songmei Li, Shubin Yang, Bin Li
Phase-change electrolytes hold great promise for sustainable energy storage technologies but are constrained by limited ionic conductivity and inefficient ion transport across phase transitions. In this work, to boost the lithium transport in polycaprolactone (PCL)-based phase-change polymer electrolyte, a novel semi-vehicle lithium transport pathway, which integrates solvent-mediated and polymer-assisted migration, has been created via a co-solvent strategy. It is demonstrated that the preferential coordination of dimethyl dodecanedioate (DDCA) and propylene carbonate (PC) attenuates the interaction between lithium ion and PCL chain, achieving continuous and rapid ion transport across phase transition. Further, the synergistic effect of linear and cyclic solvents promotes the formation of LiF-rich inorganic SEI layer, effectively stabilizing the lithium anode. The resulted electrolyte (PCL-DDCA-PC) achieves a high ionic conductivity of 3.38 × 10-4 S cm-1 and Li+ transference number of 0.84. In cell tests, the Li||Li symmetric cell exhibits stable cycling over 1000 hours at 0.05 mA cm-2. The Li||LiFePO₄ cells retain 91% capacity after 500 cycles at 0.5 C, while Li||NCM811 cells retain 80% after 200 cycles. Due to unique endothermic phase-change effect of PCL and DDCA, the obtained electrolyte enables Li//LFP pouch cells to demonstrate enhanced thermal hysteresis, reaching 100°C at a rate four times slower than those with liquid electrolytes
{"title":"Boosting the lithium transport in phase-change polymer electrolyte towards cycling stable lithium metal battery with thermal-robustness","authors":"Yulong He, Zicheng Luo, Hongfei Xu, Zehong Yuan, Songmei Li, Shubin Yang, Bin Li","doi":"10.1039/d5ta00896d","DOIUrl":"https://doi.org/10.1039/d5ta00896d","url":null,"abstract":"Phase-change electrolytes hold great promise for sustainable energy storage technologies but are constrained by limited ionic conductivity and inefficient ion transport across phase transitions. In this work, to boost the lithium transport in polycaprolactone (PCL)-based phase-change polymer electrolyte, a novel semi-vehicle lithium transport pathway, which integrates solvent-mediated and polymer-assisted migration, has been created via a co-solvent strategy. It is demonstrated that the preferential coordination of dimethyl dodecanedioate (DDCA) and propylene carbonate (PC) attenuates the interaction between lithium ion and PCL chain, achieving continuous and rapid ion transport across phase transition. Further, the synergistic effect of linear and cyclic solvents promotes the formation of LiF-rich inorganic SEI layer, effectively stabilizing the lithium anode. The resulted electrolyte (PCL-DDCA-PC) achieves a high ionic conductivity of 3.38 × 10-4 S cm-1 and Li+ transference number of 0.84. In cell tests, the Li||Li symmetric cell exhibits stable cycling over 1000 hours at 0.05 mA cm-2. The Li||LiFePO₄ cells retain 91% capacity after 500 cycles at 0.5 C, while Li||NCM811 cells retain 80% after 200 cycles. Due to unique endothermic phase-change effect of PCL and DDCA, the obtained electrolyte enables Li//LFP pouch cells to demonstrate enhanced thermal hysteresis, reaching 100°C at a rate four times slower than those with liquid electrolytes","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"121 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143832348","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
In Tae Kim, Tae Ha Kim, Seong Jun Moon, Gi Dae Park, Yoo Sei Park
Correction for ‘Yolk–shell structured microspheres consisting of CoO/CoP hetero-interfaced nanocomposites as highly active hydrogen evolution reaction electrocatalysts for AEM electrolyzer stacks’ by In Tae Kim et al., J. Mater. Chem. A, 2025, https://doi.org/10.1039/D4TA07211A.
In Tae Kim 等人在 J. Mater.Chem.A，2025，https://doi.org/10.1039/D4TA07211A。
{"title":"Correction: Yolk–shell structured microspheres consisting of CoO/CoP hetero-interfaced nanocomposites as highly active hydrogen evolution reaction electrocatalysts for AEM electrolyzer stacks","authors":"In Tae Kim, Tae Ha Kim, Seong Jun Moon, Gi Dae Park, Yoo Sei Park","doi":"10.1039/d5ta90086g","DOIUrl":"https://doi.org/10.1039/d5ta90086g","url":null,"abstract":"Correction for ‘Yolk–shell structured microspheres consisting of CoO/CoP hetero-interfaced nanocomposites as highly active hydrogen evolution reaction electrocatalysts for AEM electrolyzer stacks’ by In Tae Kim <em>et al.</em>, <em>J. Mater. Chem. A</em>, 2025, https://doi.org/10.1039/D4TA07211A.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"108 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143831979","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Hanhong Zhang, Wenjing Hou, Yuanlong Deng, Jun Song, Fan Zhang
NiOx nanoparticles are the preferred hole transport material in perovskite solar cells due to their high hole mobility, ease of fabrication, excellent stability, and suitable Fermi level for hole extraction. However, NiOx nanoparticles can undergo interfacial reactions with the perovskite active layer, potentially causing significant interface issues that limit the photovoltaic conversion efficiency and stability of perovskite solar cells. In this study, we discovered a liquid coupling agent, aluminum di(isopropoxide)acetoacetic ester chelate, which reacts with NiOx to form a hydrophilic monolayer modification through an alcoholysis process. This modification enhances both the photovoltaic conversion efficiency and stability of perovskite solar cells. The maximum efficiency of the modified perovskite solar cell reached 23.82%. Furthermore, the coupling agent is compatible with large-area coating processes. A large-area (14 cm²) perovskite solar cell module achieved an efficiency of 21.80%, retaining 97.7% of its initial performance after 600 hours under AM1.5G illumination.
{"title":"Enhancing Inverted Perovskite Solar Cells via Hydrophilic Surface Modification of NiOx Using Aluminate Coupling Agents","authors":"Hanhong Zhang, Wenjing Hou, Yuanlong Deng, Jun Song, Fan Zhang","doi":"10.1039/d5ta01516b","DOIUrl":"https://doi.org/10.1039/d5ta01516b","url":null,"abstract":"NiOx nanoparticles are the preferred hole transport material in perovskite solar cells due to their high hole mobility, ease of fabrication, excellent stability, and suitable Fermi level for hole extraction. However, NiOx nanoparticles can undergo interfacial reactions with the perovskite active layer, potentially causing significant interface issues that limit the photovoltaic conversion efficiency and stability of perovskite solar cells. In this study, we discovered a liquid coupling agent, aluminum di(isopropoxide)acetoacetic ester chelate, which reacts with NiOx to form a hydrophilic monolayer modification through an alcoholysis process. This modification enhances both the photovoltaic conversion efficiency and stability of perovskite solar cells. The maximum efficiency of the modified perovskite solar cell reached 23.82%. Furthermore, the coupling agent is compatible with large-area coating processes. A large-area (14 cm²) perovskite solar cell module achieved an efficiency of 21.80%, retaining 97.7% of its initial performance after 600 hours under AM1.5G illumination.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"7 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143832350","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Xueli Zhang, Shihao Ding, Qianqian Shen, Shilong Feng, Jinlong Li, Zhe Sun, Chengkun Lei, Jinbo Xue, Min Liu
The development of inexpensive and stable hydrogen evolution reaction (HER)/oxygen evolution reaction (OER) bifunctional electrocatalysts is extremely important to advance the commercial application of alkaline water electrolysis (AWE). However, the majority of bifunctional catalysts exhibit optimal activity in only one reaction, leading to suboptimal overall water splitting efficiency. The development of a satisfactory bifunctional catalyst capable of simultaneously accelerating both HER and OER kinetics remains an ongoing challenge. Here, we report efficient bifunctional electrocatalytic water splitting by constructing long-range ordered oxygen vacancies in hematite nanobelt arrays. Notably, HNBs-30 with long-range ordered oxygen vacancies exhibits lower OER (317 mV @ 10 mA cm−2, 369 mV @ 100 mA cm−2) and HER (178 mV @ 10 mA cm−2, 321 mV @ 100 mA cm−2) overpotentials, and exhibits a low overpotential of 2.22 V and long-term stability of 40 hours at 100 mA cm−2 in overall water splitting. This study shows that long-range ordered oxygen vacancies not only optimize the adsorption/desorption kinetics of intermediates, but also establish a highly efficient conduit for charge transport, which can simultaneously accelerate the kinetics of HER and OER. This is a key factor in HNBs-30 achieving bifunctional and high catalytic activity.
{"title":"Hematite nanobelts with ordered oxygen vacancies for bifunctional electrocatalytic water splitting","authors":"Xueli Zhang, Shihao Ding, Qianqian Shen, Shilong Feng, Jinlong Li, Zhe Sun, Chengkun Lei, Jinbo Xue, Min Liu","doi":"10.1039/d5ta01217a","DOIUrl":"https://doi.org/10.1039/d5ta01217a","url":null,"abstract":"The development of inexpensive and stable hydrogen evolution reaction (HER)/oxygen evolution reaction (OER) bifunctional electrocatalysts is extremely important to advance the commercial application of alkaline water electrolysis (AWE). However, the majority of bifunctional catalysts exhibit optimal activity in only one reaction, leading to suboptimal overall water splitting efficiency. The development of a satisfactory bifunctional catalyst capable of simultaneously accelerating both HER and OER kinetics remains an ongoing challenge. Here, we report efficient bifunctional electrocatalytic water splitting by constructing long-range ordered oxygen vacancies in hematite nanobelt arrays. Notably, HNBs-30 with long-range ordered oxygen vacancies exhibits lower OER (317 mV @ 10 mA cm<small><sup>−2</sup></small>, 369 mV @ 100 mA cm<small><sup>−2</sup></small>) and HER (178 mV @ 10 mA cm<small><sup>−2</sup></small>, 321 mV @ 100 mA cm<small><sup>−2</sup></small>) overpotentials, and exhibits a low overpotential of 2.22 V and long-term stability of 40 hours at 100 mA cm<small><sup>−2</sup></small> in overall water splitting. This study shows that long-range ordered oxygen vacancies not only optimize the adsorption/desorption kinetics of intermediates, but also establish a highly efficient conduit for charge transport, which can simultaneously accelerate the kinetics of HER and OER. This is a key factor in HNBs-30 achieving bifunctional and high catalytic activity.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"8 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143832347","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Investigating a single multifunctional electrode in an integrated device, such as self-powered overall water splitting (OWS), is extremely valuable since it may substantially decrease the system complexity and expense. Hence, a full rice-spike-like 400N-CDs/FeNi-TDC nanoarray combining N-hybridized carbon dots (N-CDs) and FeNi-TDC with 2,5-thiophenedicarboxylic acid (H2TDC) as ligands is constructed on the surface of a nickel foam by a one-pot solvothermal method for OWS and supercapacitor applications. Based on interface-heterojunction engineering, the morphology and electronic environment at the active sites of the nanomaterial successfully controlled by N-CDs and the heterojunction synergistically promoted efficient catalysis. The optimized 400N-CDs/FeNi-TDC electrode exhibits a 209 mV overpotential and a Tafel slope of 18.91 mV dec−1 at 10 mA cm−2 during the oxygen evolution reaction (OER) activity, as well as a low overpotential of 99 mV to reach 10 mA cm−2 with a Tafel slope of 77.01 mV dec−1 in the hydrogen evolution reaction (HER). As the positive electrode of the supercapacitor, the high specific capacitance of 400N-CDs/FeNi-TDC is 2388 F g−1 at 1 A g−1. The assembled self-powered OWS device uses the 400N-CDs/FeNi-TDC‖AC/NF with pre-charged 3 V as the power supply to achieve simultaneous green hydrogen and oxygen production for ∼4 min. This research provides a new platform to build state-of-the-art and sustainable energy conversion and storage devices.
{"title":"In situ formation of heterojunction of thiophene-based metal–organic frameworks with carbon dots for efficient overall water splitting and supercapacitor applications","authors":"Qianqian Wang, Xiaoyan Ma, Ran Bi, Xiangpan Hu, Senyang Song, Pengcheng Ma, Fang Chen","doi":"10.1039/d4ta08523j","DOIUrl":"https://doi.org/10.1039/d4ta08523j","url":null,"abstract":"Investigating a single multifunctional electrode in an integrated device, such as self-powered overall water splitting (OWS), is extremely valuable since it may substantially decrease the system complexity and expense. Hence, a full rice-spike-like 400N-CDs/FeNi-TDC nanoarray combining N-hybridized carbon dots (N-CDs) and FeNi-TDC with 2,5-thiophenedicarboxylic acid (H<small><sub>2</sub></small>TDC) as ligands is constructed on the surface of a nickel foam by a one-pot solvothermal method for OWS and supercapacitor applications. Based on interface-heterojunction engineering, the morphology and electronic environment at the active sites of the nanomaterial successfully controlled by N-CDs and the heterojunction synergistically promoted efficient catalysis. The optimized 400N-CDs/FeNi-TDC electrode exhibits a 209 mV overpotential and a Tafel slope of 18.91 mV dec<small><sup>−1</sup></small> at 10 mA cm<small><sup>−2</sup></small> during the oxygen evolution reaction (OER) activity, as well as a low overpotential of 99 mV to reach 10 mA cm<small><sup>−2</sup></small> with a Tafel slope of 77.01 mV dec<small><sup>−1</sup></small> in the hydrogen evolution reaction (HER). As the positive electrode of the supercapacitor, the high specific capacitance of 400N-CDs/FeNi-TDC is 2388 F g<small><sup>−1</sup></small> at 1 A g<small><sup>−1</sup></small>. The assembled self-powered OWS device uses the 400N-CDs/FeNi-TDC‖AC/NF with pre-charged 3 V as the power supply to achieve simultaneous green hydrogen and oxygen production for ∼4 min. This research provides a new platform to build state-of-the-art and sustainable energy conversion and storage devices.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"39 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143832339","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Min Woo Kim, Jong Min Lee, Chi-Young Jung, Jung-Eun Cha, Kwang Shik Myung, Nam Jin Lee, Nam Dong Kim, Jae Young Jung
Enhancing the durability of platinum catalysts in proton exchange membrane fuel cells (PEMFCs) remains a key challenge for long-haul truck applications. In this study, we employed a commercialized high-surface-area carbon support and performed thermal annealing under oxidizing/reducing conditions to precisely control the oxygen functional groups on its surface. Subsequently, platinum nanoparticles (Pt NPs) were uniformly dispersed on the carbon support via a polyol method. We systematically investigated the Pt NPs/carbon interface effect using advanced spectroscopic techniques combined with electrochemical surface analyses, while isolating the effects of Pt location and pore structure. Consequently, we significantly improved the durability of the platinum catalyst, with mass activity retention increasing from 40.9% to 78.6% of initial performance (0.393–0.403 A mgPt−1), and the electrochemical surface area (ECSA) rising from 57.9% to 84.2% of initial ECSA values (95–97 m2 gPt−1). These improvements were achieved while maintaining highly precise initial parameters. Through extensive material characterization, we demonstrated that the improved durability of the platinum catalyst is attributed to the increased binding energy between the oxygen functional groups and Pt nanoparticles (NPs), as well as the suppression of Pt ionization. This study highlights the crucial role of carbon supports in fuel cells and provides guidelines for optimal design, paving the way for platinum catalysts intended for long-range fuel cell applications in areas such as ecofriendly hydrogen vehicles and distributed power generation.
{"title":"Thermally driven oxygen functionalization for durable Pt electrocatalysts in the oxygen reduction reaction","authors":"Min Woo Kim, Jong Min Lee, Chi-Young Jung, Jung-Eun Cha, Kwang Shik Myung, Nam Jin Lee, Nam Dong Kim, Jae Young Jung","doi":"10.1039/d5ta01939g","DOIUrl":"https://doi.org/10.1039/d5ta01939g","url":null,"abstract":"Enhancing the durability of platinum catalysts in proton exchange membrane fuel cells (PEMFCs) remains a key challenge for long-haul truck applications. In this study, we employed a commercialized high-surface-area carbon support and performed thermal annealing under oxidizing/reducing conditions to precisely control the oxygen functional groups on its surface. Subsequently, platinum nanoparticles (Pt NPs) were uniformly dispersed on the carbon support <em>via</em> a polyol method. We systematically investigated the Pt NPs/carbon interface effect using advanced spectroscopic techniques combined with electrochemical surface analyses, while isolating the effects of Pt location and pore structure. Consequently, we significantly improved the durability of the platinum catalyst, with mass activity retention increasing from 40.9% to 78.6% of initial performance (0.393–0.403 A mg<small><sub>Pt</sub></small><small><sup>−1</sup></small>), and the electrochemical surface area (ECSA) rising from 57.9% to 84.2% of initial ECSA values (95–97 m<small><sup>2</sup></small> g<small><sub>Pt</sub></small><small><sup>−1</sup></small>). These improvements were achieved while maintaining highly precise initial parameters. Through extensive material characterization, we demonstrated that the improved durability of the platinum catalyst is attributed to the increased binding energy between the oxygen functional groups and Pt nanoparticles (NPs), as well as the suppression of Pt ionization. This study highlights the crucial role of carbon supports in fuel cells and provides guidelines for optimal design, paving the way for platinum catalysts intended for long-range fuel cell applications in areas such as ecofriendly hydrogen vehicles and distributed power generation.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"74 5 Pt 1 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143832341","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Due to the complexity of insoluble Li2S2-Li2S conversion, few descriptors exist to correlate the catalytic performance and the underlying electronic structures of a given catalyst, which inhibits the development of lithium−sulfur catalysts. In this article, we employ the cluster expansion method to select 17 optimal structures for TaXTi(1-X)S2 (0≤X≤1) and apply density functional theory calculations to probe the electronic structures and the conversion of Li2S2 to Li2S relationships across different doping concentrations. We found the simultaneous pathway is most possible in propose five possible reaction pathways. Notably, we identify Ta0.38Ti0.62S2 as a promising candidate for electrocatalytic applications in the conversion from Li2S2 to Li2S. Furthermore, our study analyzes the charge transfer of Li2S2(QLi2S2), the electronegative difference(ΔX), the adsorption energy of Li2S(EaLi2S), and work function(WF) significantly influence the conversion process from Li2S2 to Li2S by machine learning based on various descriptors. This research contributes to a deeper theoretical understanding of the complex mechanisms underlying the Li2S2-Li2S conversion and provides valuable insights into the rational design of sulfur redox catalysts.
{"title":"Density Functional Theory Studies on Tuning TaXTi(1-X)S2 For Insoluble Li2S2-Li2S Conversion in Lithium-Sulfur Batteries","authors":"Jinyan Chen, Shuai Zhao, Yuhan Wang, Ruiyu Hao, Chao Gao, Jianhua Hou","doi":"10.1039/d5ta01770j","DOIUrl":"https://doi.org/10.1039/d5ta01770j","url":null,"abstract":"Due to the complexity of insoluble Li2S2-Li2S conversion, few descriptors exist to correlate the catalytic performance and the underlying electronic structures of a given catalyst, which inhibits the development of lithium−sulfur catalysts. In this article, we employ the cluster expansion method to select 17 optimal structures for TaXTi(1-X)S2 (0≤X≤1) and apply density functional theory calculations to probe the electronic structures and the conversion of Li2S2 to Li2S relationships across different doping concentrations. We found the simultaneous pathway is most possible in propose five possible reaction pathways. Notably, we identify Ta0.38Ti0.62S2 as a promising candidate for electrocatalytic applications in the conversion from Li2S2 to Li2S. Furthermore, our study analyzes the charge transfer of Li2S2(QLi2S2), the electronegative difference(ΔX), the adsorption energy of Li2S(EaLi2S), and work function(WF) significantly influence the conversion process from Li2S2 to Li2S by machine learning based on various descriptors. This research contributes to a deeper theoretical understanding of the complex mechanisms underlying the Li2S2-Li2S conversion and provides valuable insights into the rational design of sulfur redox catalysts.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"15 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-04-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143832352","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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