Charge transfer at the electrode/electrolyte interface and mass transfer within the electrode are the two main factors affecting the high-rate performance of O3-type layered oxide cathodes for sodium-ion batteries. Here a multidimensional lanthurization strategy is proposed to construct the surface LaCrO3 heterostructure and create a Cr─O─La configuration for O3-type NaCrO2. The electrified heterogeneous LaCrO3 induces a built-in electric field to accelerate charge transfer at the interface. Meanwhile, the Cr─O─La configuration in the transition metal layer leads to local charge aggregation, weakens the interaction force between Na─O, and reduces the Na+ migration barrier. This strategy significantly improves the electrochemical reaction kinetics and the structural reversibility of the layered oxide cathode. As a result, the designed stoichiometric ratio Na0.94Cr0.98La0.02O2 electrode exhibits remarkable rate performance (101.8 mAh g−1 at 40 C) as well as outstanding cycling stability (83.1% capacity retention at 20 C for 2000 cycles) in a half-cell, along with a competitive full battery performance (89.3% after 500 cycles at 2 C). This study provides a promising route to achieve capacity presentation and retention of layered oxide cathode materials at high-rate.
{"title":"Configuration Design and Interface Reconstruction to Realize the Superior High-Rate Performance for Sodium Layered Oxide Cathodes","authors":"Jiandong Zhang, Zhaoshi Yu, Yanbin Zhu, Jingyao Cai, Muqin Wang, Pengkun Gao, Yali Zhang, Naiqing Zhang, Deyu Wang, Yan Shen, Mingkui Wang","doi":"10.1002/aenm.202405951","DOIUrl":"https://doi.org/10.1002/aenm.202405951","url":null,"abstract":"Charge transfer at the electrode/electrolyte interface and mass transfer within the electrode are the two main factors affecting the high-rate performance of O3-type layered oxide cathodes for sodium-ion batteries. Here a multidimensional lanthurization strategy is proposed to construct the surface LaCrO<sub>3</sub> heterostructure and create a Cr─O─La configuration for O3-type NaCrO<sub>2</sub>. The electrified heterogeneous LaCrO<sub>3</sub> induces a built-in electric field to accelerate charge transfer at the interface. Meanwhile, the Cr─O─La configuration in the transition metal layer leads to local charge aggregation, weakens the interaction force between Na─O, and reduces the Na<sup>+</sup> migration barrier. This strategy significantly improves the electrochemical reaction kinetics and the structural reversibility of the layered oxide cathode. As a result, the designed stoichiometric ratio Na<sub>0.94</sub>Cr<sub>0.98</sub>La<sub>0.02</sub>O<sub>2</sub> electrode exhibits remarkable rate performance (101.8 mAh g<sup>−1</sup> at 40 C) as well as outstanding cycling stability (83.1% capacity retention at 20 C for 2000 cycles) in a half-cell, along with a competitive full battery performance (89.3% after 500 cycles at 2 C). This study provides a promising route to achieve capacity presentation and retention of layered oxide cathode materials at high-rate.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"63 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143385849","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Wenbo Zhao, Jipeng Chen, Ximeng Liu, Yong Gao, Jie Pu, Qinghe Cao, Ting Meng, Abdelnaby M. Elshahawy, Salah A. Makhlouf, Cao Guan
The design of efficient oxygen reductionreaction (ORR) catalyst with fast kinetics is crucial for high-performance Zn–air batteries but remains a challenge. Herein, inspired by the oxidative respiratory chain of prokaryotes, an ORR electrocatalyst is reported by mimicking the microstructure of Staphylococcus aureus and simitaneously utilizing this low-cost cell as the precursor. The catalyst consists of MnO2/Co2P nanocomposites support on Staphylococcus aureus-derived hollow spherical carbon, which not only accelerates electron transfer for improved intrinsic reaction kinetics, but also creates an OH− concentration gradient for enhanced mass transfer efficiency. Such bio-inspired and derived ORR catalyst enables rechargeable Zn–air batteries with ultra-long cycling stability of more than 2800 h at a high capacity of 810.3 mAh g−1, which is superior among the reported bio-derived oxygen catalysts. A flexible Zn–air battery based on the bio-inspired and derived catalyst is also assembled, and it well integrates with a wireless flexible electronic skin.
{"title":"Prokaryote-Inspired and Derived Oxygen Reduction Electrocatalysts for Ultra-Long-Life Zn–Air Batteries","authors":"Wenbo Zhao, Jipeng Chen, Ximeng Liu, Yong Gao, Jie Pu, Qinghe Cao, Ting Meng, Abdelnaby M. Elshahawy, Salah A. Makhlouf, Cao Guan","doi":"10.1002/aenm.202405594","DOIUrl":"https://doi.org/10.1002/aenm.202405594","url":null,"abstract":"The design of efficient oxygen reductionreaction (ORR) catalyst with fast kinetics is crucial for high-performance Zn–air batteries but remains a challenge. Herein, inspired by the oxidative respiratory chain of prokaryotes, an ORR electrocatalyst is reported by mimicking the microstructure of Staphylococcus aureus and simitaneously utilizing this low-cost cell as the precursor. The catalyst consists of MnO<sub>2</sub>/Co<sub>2</sub>P nanocomposites support on Staphylococcus aureus-derived hollow spherical carbon, which not only accelerates electron transfer for improved intrinsic reaction kinetics, but also creates an OH<sup>−</sup> concentration gradient for enhanced mass transfer efficiency. Such bio-inspired and derived ORR catalyst enables rechargeable Zn–air batteries with ultra-long cycling stability of more than 2800 h at a high capacity of 810.3 mAh g<sup>−1</sup>, which is superior among the reported bio-derived oxygen catalysts. A flexible Zn–air battery based on the bio-inspired and derived catalyst is also assembled, and it well integrates with a wireless flexible electronic skin.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"1 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143385845","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Lin Wang, Neelam Sunariwal, Yufang He, Do-hoon Kim, Dong-hee Yeon, Yan Zeng, Jordi Cabana, Bin Ouyang
High entropy disordered rocksalt (HE-DRX) Li-ion battery positive electrodes have gained attention as a potential alternative to commercialized positive electrodes, aiming to eliminate or minimize the use of Ni/Co while maintaining competitive electrochemical performance. Despite their potential, understanding the intricate elemental stability across the vast HE-DRX chemical landscape remains a significant challenge. In this study, we tackle this challenge by conducting a comprehensive data-driven phase diagram analysis of 18810 potential HE-DRX compositions, each featuring common Li and F stoichiometries. Leveraging a charge balance algorithm, we systematically explore redox stability and phase stability, unveiling critical insights into chemical stability rules within the HE-DRX design space. The analysis also uncovers untapped potential of Cu as redox-active centers, with Sb and Sn contributing as stable charge compensators. The utilization of these elements is seldom reported in the literature but has been validated by the successful experimental synthesis of materials Li21Zr3Ti3Mn2Fe5Cu2O36 and Li21Mn2Ti3Fe5Cu2Sn3O36.
{"title":"Elemental Stability Rules for High Entropy Disordered Rocksalt Type Li-Ion Battery Positive Electrodes","authors":"Lin Wang, Neelam Sunariwal, Yufang He, Do-hoon Kim, Dong-hee Yeon, Yan Zeng, Jordi Cabana, Bin Ouyang","doi":"10.1002/aenm.202404982","DOIUrl":"https://doi.org/10.1002/aenm.202404982","url":null,"abstract":"High entropy disordered rocksalt (HE-DRX) Li-ion battery positive electrodes have gained attention as a potential alternative to commercialized positive electrodes, aiming to eliminate or minimize the use of Ni/Co while maintaining competitive electrochemical performance. Despite their potential, understanding the intricate elemental stability across the vast HE-DRX chemical landscape remains a significant challenge. In this study, we tackle this challenge by conducting a comprehensive data-driven phase diagram analysis of 18810 potential HE-DRX compositions, each featuring common Li and F stoichiometries. Leveraging a charge balance algorithm, we systematically explore redox stability and phase stability, unveiling critical insights into chemical stability rules within the HE-DRX design space. The analysis also uncovers untapped potential of Cu as redox-active centers, with Sb and Sn contributing as stable charge compensators. The utilization of these elements is seldom reported in the literature but has been validated by the successful experimental synthesis of materials Li<sub>21</sub>Zr<sub>3</sub>Ti<sub>3</sub>Mn<sub>2</sub>Fe<sub>5</sub>Cu<sub>2</sub>O<sub>36</sub> and Li<sub>21</sub>Mn<sub>2</sub>Ti<sub>3</sub>Fe<sub>5</sub>Cu<sub>2</sub>Sn<sub>3</sub>O<sub>36</sub>.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"19 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143385852","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Huan Liu, Chenghan Yang, Tong Bian, Huijun Yu, Yuming Zhou, Yiwei Zhang, Li Sun
Enhancing the selectivity of C2 products and revealing the reaction mechanisms in CO2 electroreduction reaction (CO2RR) remain challenging. Regulating the interphases in catalysts is one of the most promising pathways. Herein, the interphases between copper (Cu) and tin (Sn) oxides are regulated by controlling the degree of reduction during the self-assembly process, which exhibits obvious different selectivity to ethylene and ethanol, respectively. The interphase in Cu-SnO2 exhibits selectivity to ethanol as high as 74.6%, while the interphase in Cu2O-SnO2 shows selectivity to ethylene as high as 71.4% at –0.6 V versus RHE. In situ Fourier-transform infrared spectroscopy measurements and density functional theory calculations demonstrate that the interphase in Cu-SnO2 shows strong electron interaction, preferentially forming the key *COH intermediates for asymmetrical C─C coupling to produce ethanol. In contrast, Cu2O-SnO2 possesses oxygen vacancies at both sites, thus enriching *CO intermediates for symmetrical C─C coupling to produce ethylene at the interphase. The findings in this work offer an advanced strategy by regulating the interphases to adjust C2 selectivity in CO2RR.
{"title":"Adjustable Selectivity for CO2 Electroreduction to Ethylene or Ethanol by Regulating Interphases Between Copper and Tin Oxides","authors":"Huan Liu, Chenghan Yang, Tong Bian, Huijun Yu, Yuming Zhou, Yiwei Zhang, Li Sun","doi":"10.1002/aenm.202405658","DOIUrl":"https://doi.org/10.1002/aenm.202405658","url":null,"abstract":"Enhancing the selectivity of C<sub>2</sub> products and revealing the reaction mechanisms in CO<sub>2</sub> electroreduction reaction (CO<sub>2</sub>RR) remain challenging. Regulating the interphases in catalysts is one of the most promising pathways. Herein, the interphases between copper (Cu) and tin (Sn) oxides are regulated by controlling the degree of reduction during the self-assembly process, which exhibits obvious different selectivity to ethylene and ethanol, respectively. The interphase in Cu-SnO<sub>2</sub> exhibits selectivity to ethanol as high as 74.6%, while the interphase in Cu<sub>2</sub>O-SnO<sub>2</sub> shows selectivity to ethylene as high as 71.4% at –0.6 V versus RHE. In situ Fourier-transform infrared spectroscopy measurements and density functional theory calculations demonstrate that the interphase in Cu-SnO<sub>2</sub> shows strong electron interaction, preferentially forming the key *COH intermediates for asymmetrical C─C coupling to produce ethanol. In contrast, Cu<sub>2</sub>O-SnO<sub>2</sub> possesses oxygen vacancies at both sites, thus enriching *CO intermediates for symmetrical C─C coupling to produce ethylene at the interphase. The findings in this work offer an advanced strategy by regulating the interphases to adjust C<sub>2</sub> selectivity in CO<sub>2</sub>RR.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"60 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143385846","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yanan Gao, Bo Ouyang, Yuan Shen, Wei Wen, Junxiang Wang, Mingzhe Wang, Yiqiang Sun, Kun Xu
Developing highly active and CO-resistant Ru-based catalysts for the alkaline hydrogen oxidation reaction (HOR) can advance the large-scale application of alkaline hydrogen fuel cells but remains a huge challenge. Herein, a pure phase W2C supported Ru cluster catalyst (Ru/W2C) is successfully synthesized through a one-step carburization method. It is found that the charge transfer from W2C to the strongly anchored Ru clusters forms the electron-rich Ruδ− sites and electron-deficient Wδ+ sites, which significantly weakens the adsorption strength of *H and *CO, strengthens the binding of *OH and improves the water connectivity in the electric double layer. The Ru/W2C catalyst shows superior mass activity (2163 mA mgPGM−1) in alkaline HOR, which is 12.52 and 20.62 times higher than that for Pt/C and Ru/C, respectively. Owing to the weak adsorption and fast removal rate of CO, the Ru/W2C exhibits outstanding CO tolerance, with 88% of the initial activity being retained in the durability test, whereas the Ru/C and Pt/C suffer from severe deactivation. These findings may guide the design of advanced alkaline HOR catalysts based on the pure phase tungsten carbide.
{"title":"Electron-Rich Ru Clusters Anchored on Pure Phase W2C Enables Highly Active and CO-Resistant Alkaline Hydrogen Oxidation","authors":"Yanan Gao, Bo Ouyang, Yuan Shen, Wei Wen, Junxiang Wang, Mingzhe Wang, Yiqiang Sun, Kun Xu","doi":"10.1002/aenm.202406114","DOIUrl":"https://doi.org/10.1002/aenm.202406114","url":null,"abstract":"Developing highly active and CO-resistant Ru-based catalysts for the alkaline hydrogen oxidation reaction (HOR) can advance the large-scale application of alkaline hydrogen fuel cells but remains a huge challenge. Herein, a pure phase W<sub>2</sub>C supported Ru cluster catalyst (Ru/W<sub>2</sub>C) is successfully synthesized through a one-step carburization method. It is found that the charge transfer from W<sub>2</sub>C to the strongly anchored Ru clusters forms the electron-rich Ru<sup>δ−</sup> sites and electron-deficient W<sup>δ+</sup> sites, which significantly weakens the adsorption strength of <sup>*</sup>H and <sup>*</sup>CO, strengthens the binding of <sup>*</sup>OH and improves the water connectivity in the electric double layer. The Ru/W<sub>2</sub>C catalyst shows superior mass activity (2163 mA mg<sub>PGM</sub><sup>−1</sup>) in alkaline HOR, which is 12.52 and 20.62 times higher than that for Pt/C and Ru/C, respectively. Owing to the weak adsorption and fast removal rate of CO, the Ru/W<sub>2</sub>C exhibits outstanding CO tolerance, with 88% of the initial activity being retained in the durability test, whereas the Ru/C and Pt/C suffer from severe deactivation. These findings may guide the design of advanced alkaline HOR catalysts based on the pure phase tungsten carbide.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"55 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143385848","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The acid-base reaction of CO2 with hydroxide ions to (bi)carbonate anions at the cathode of alkaline exchange membrane (AEM) CO2 electrolyzer has detrimental impact on their performance. (Bi)carbonate buffers the local cathode pH, and in combination with metal cations, may lead to precipitation of salts at the cathode. This non-electrochemical conversion of CO2 significantly reduces the CO2 utilization efficiency and limits the CO2 single pass conversion of AEM CO2 electrolyzer to 50% if CO is desired. Acidic metal cation-free CO2 electrolysis has the potential to address and mitigate these problems. Here, CO2 valorization is demonstrated at faradaic CO efficiencies (FE) of up to 80% FECO in forward-bias BPM cell architectures using actual neutral pure water feeding at the anode. This study demonstrates how immobilized anion exchange ionomer layers thereby facilitate the metal cation-free CO2 valorization thanks to their positively charged functional NR4 groups. Unlike metal cations, the immobilized positively charged groups are not washed out of the reactor. This study shows that careful design of the distribution and location of the anion exchange ionomer molecules within the Gas Diffusion Electrode is key to efficient CO2-to-CO electrolyzer cell.
{"title":"Efficient Forward-Bias Bipolar Membrane CO2 Electrolysis in Absence of Metal Cations","authors":"Sven Brückner, Wen Ju, Peter Strasser","doi":"10.1002/aenm.202500186","DOIUrl":"https://doi.org/10.1002/aenm.202500186","url":null,"abstract":"The acid-base reaction of CO<sub>2</sub> with hydroxide ions to (bi)carbonate anions at the cathode of alkaline exchange membrane (AEM) CO<sub>2</sub> electrolyzer has detrimental impact on their performance. (Bi)carbonate buffers the local cathode pH, and in combination with metal cations, may lead to precipitation of salts at the cathode. This non-electrochemical conversion of CO<sub>2</sub> significantly reduces the CO<sub>2</sub> utilization efficiency and limits the CO<sub>2</sub> single pass conversion of AEM CO<sub>2</sub> electrolyzer to 50% if CO is desired. Acidic metal cation-free CO<sub>2</sub> electrolysis has the potential to address and mitigate these problems. Here, CO<sub>2</sub> valorization is demonstrated at faradaic CO efficiencies (FE) of up to 80% FE<sub>CO</sub> in forward-bias BPM cell architectures using actual neutral pure water feeding at the anode. This study demonstrates how immobilized anion exchange ionomer layers thereby facilitate the metal cation-free CO<sub>2</sub> valorization thanks to their positively charged functional NR<sub>4</sub> groups. Unlike metal cations, the immobilized positively charged groups are not washed out of the reactor. This study shows that careful design of the distribution and location of the anion exchange ionomer molecules within the Gas Diffusion Electrode is key to efficient CO<sub>2</sub>-to-CO electrolyzer cell.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"29 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143375628","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Polymeric carbon nitrides (PCNs) exhibit intriguing optical properties and exceptional performance in (photo)catalysis, optoelectronics, and energy storage. Nevertheless, the intricate phenomena involving light absorption, formation of long-lived excitons, photo-charging, and photochemical processes observed in PCNs remain poorly understood. This theoretical investigation elucidates the origin of distinct dark and bright excitons, their stability and lifetimes, and their correlation with the microstructural attributes of PCNs. Based on these results, the decisive role of dark excitons in photocatalytic reactivity is proposed, which underlies the experimentally observed differences in the photocatalytic performance of various PCN derivatives. This study thus establishes novel insights into the factors governing the light-driven processes in PCNs that can provide essential guidelines for rational design of PCNs with enhanced performance.
{"title":"Structural Influence on Exciton Formation and the Critical Role of Dark Excitons in Polymeric Carbon Nitrides","authors":"Changbin Im, Radim Beranek, Timo Jacob","doi":"10.1002/aenm.202405549","DOIUrl":"https://doi.org/10.1002/aenm.202405549","url":null,"abstract":"Polymeric carbon nitrides (PCNs) exhibit intriguing optical properties and exceptional performance in (photo)catalysis, optoelectronics, and energy storage. Nevertheless, the intricate phenomena involving light absorption, formation of long-lived excitons, photo-charging, and photochemical processes observed in PCNs remain poorly understood. This theoretical investigation elucidates the origin of distinct dark and bright excitons, their stability and lifetimes, and their correlation with the microstructural attributes of PCNs. Based on these results, the decisive role of dark excitons in photocatalytic reactivity is proposed, which underlies the experimentally observed differences in the photocatalytic performance of various PCN derivatives. This study thus establishes novel insights into the factors governing the light-driven processes in PCNs that can provide essential guidelines for rational design of PCNs with enhanced performance.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"12 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143375597","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Ao Hu, Chenghao Yang, Yitong Li, Kaisheng Xia, Yunfeng Tian, Jian Pu, Bo Chi
Reversible proton ceramic cells (R-PCCs) offer a transformative solution for dual functionality in power generation and energy storage. However, their potential is currently obstacles by the lack of high-performance air electrodes combining high electrocatalytic activity with durability. Here, an innovative air electrode composed of high-entropy driven self-assembled xNiO-Pr0.2La0.2Ba0.2Sr0.2Ca0.2Fe0.8Ni0.2−xO3−δ (N-XFN) composites is presented, which result from the unique lattice distortion effects inherent in high-entropy perovskites. The experimental results coupled with density functional theory (DFT) calculations verify that the lattice distortion at the high-entropy A-site significantly induces NiO nanoparticles exsolved from the B-site, promoting the formation of a biphasic composite structure that dramatically increases the electrochemical active sites. Remarkably, R-PCCs using the N-XFN composite air electrode achieve an impressive peak power density of 1.30 W cm−2 in fuel cell mode and a current density of -2.52 A cm−2 at 1.3 V in electrolysis mode at 650 °C. In addition, the cells show excellent stability with reversibility over 830 h, including 500 h in electrolysis mode and 330 h in reversible operation at 650 °C. This research provides important insights into the design of high-entropy perovskites, paving the way for advanced R-PCCs technology.
{"title":"High-Entropy Driven Self-Assembled Dual-phase Composite Air Electrodes with Enhanced Performance and Stability for Reversible Protonic Ceramic Cells","authors":"Ao Hu, Chenghao Yang, Yitong Li, Kaisheng Xia, Yunfeng Tian, Jian Pu, Bo Chi","doi":"10.1002/aenm.202405466","DOIUrl":"https://doi.org/10.1002/aenm.202405466","url":null,"abstract":"Reversible proton ceramic cells (R-PCCs) offer a transformative solution for dual functionality in power generation and energy storage. However, their potential is currently obstacles by the lack of high-performance air electrodes combining high electrocatalytic activity with durability. Here, an innovative air electrode composed of high-entropy driven self-assembled xNiO-Pr<sub>0.2</sub>La<sub>0.2</sub>Ba<sub>0.2</sub>Sr<sub>0.2</sub>Ca<sub>0.2</sub>Fe<sub>0.8</sub>Ni<sub>0.2−x</sub>O<sub>3−δ</sub> (N-XFN) composites is presented, which result from the unique lattice distortion effects inherent in high-entropy perovskites. The experimental results coupled with density functional theory (DFT) calculations verify that the lattice distortion at the high-entropy A-site significantly induces NiO nanoparticles exsolved from the B-site, promoting the formation of a biphasic composite structure that dramatically increases the electrochemical active sites. Remarkably, R-PCCs using the N-XFN composite air electrode achieve an impressive peak power density of 1.30 W cm<sup>−2</sup> in fuel cell mode and a current density of -2.52 A cm<sup>−2</sup> at 1.3 V in electrolysis mode at 650 °C. In addition, the cells show excellent stability with reversibility over 830 h, including 500 h in electrolysis mode and 330 h in reversible operation at 650 °C. This research provides important insights into the design of high-entropy perovskites, paving the way for advanced R-PCCs technology.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"1 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143375598","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yuou Li, Ke Wang, Zijian Wang, Xiaomei Wang, Xiang Chu, Rui Zhang, Shuyan Song, Hongjie Zhang, Xiao Wang
Ammonia decomposition reaction (ADR) has been extensively used to generate clear hydrogen in industry. Despite ruthenium (Ru) being the most active catalyst component for ADR, its exceptionally high price imposes severe limitations on its large-scale application. Therefore, the development of cost-effective and robust noble-metal-free ADR catalysts is highly desired, but it remains a challenge. Herein, a spray pyrolysis-assisted method is reported for the ultra-fast synthesis of strongly coupled composite oxide supports and transition metal alloy centers. The optimized catalyst, La0.75Sr0.25(FeCoNi)1.7O3-δ, exhibits outstanding ADR performance, achieving ≈98% ammonia conversion at 600 °C with remarkable stability over a period of 150 h. Further investigations reveal that the composite oxide support is enriched with numerous medium to strong basic sites. These sites play a crucial role in transferring electrons to the supported transition metal alloy, thus contributing to the rapid recombination and desorption of nitrogen atoms.
{"title":"Ultra-Fast Synthesis of Composite Oxide-Supported Transition Metal Alloy as an Advanced Catalyst for Ammonia Decomposition","authors":"Yuou Li, Ke Wang, Zijian Wang, Xiaomei Wang, Xiang Chu, Rui Zhang, Shuyan Song, Hongjie Zhang, Xiao Wang","doi":"10.1002/aenm.202405296","DOIUrl":"https://doi.org/10.1002/aenm.202405296","url":null,"abstract":"Ammonia decomposition reaction (ADR) has been extensively used to generate clear hydrogen in industry. Despite ruthenium (Ru) being the most active catalyst component for ADR, its exceptionally high price imposes severe limitations on its large-scale application. Therefore, the development of cost-effective and robust noble-metal-free ADR catalysts is highly desired, but it remains a challenge. Herein, a spray pyrolysis-assisted method is reported for the ultra-fast synthesis of strongly coupled composite oxide supports and transition metal alloy centers. The optimized catalyst, La<sub>0.75</sub>Sr<sub>0.25</sub>(FeCoNi)<sub>1.7</sub>O<sub>3-δ,</sub> exhibits outstanding ADR performance, achieving ≈98% ammonia conversion at 600 °C with remarkable stability over a period of 150 h. Further investigations reveal that the composite oxide support is enriched with numerous medium to strong basic sites. These sites play a crucial role in transferring electrons to the supported transition metal alloy, thus contributing to the rapid recombination and desorption of nitrogen atoms.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"26 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143375596","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Xiaoyang He, Shujie Xue, Xuan Liu, Dengke Xiong, Xin Xiao, Deli Wu, Jianying Wang, Qiang Xu, Zuofeng Chen
The rechargeable Zn-redox battery represents a promising, efficient, and sustainable energy storage technology. Herein, a novel 4-nitrobenzyl alcohol (4-NBA)-assisted rechargeable Zn-redox battery, driven by NiSe─Cu2Se/NF bifunctional electrocatalysts is developed. The different redox activities of ─NO2 and ─OH groups in 4-NBA allow redox conversion for chemical production during the whole discharge/charge process, maximizing the economic value of battery technologies. Detailed charge analyses indicate that the internal electric field within the NiSe─Cu2Se heterostructure modulates the d-band center, optimizes the adsorption/desorption strength of intermediates, and reduces the reaction energy barriers during the redox conversion of 4-NBA. This bifunctional NiSe─Cu2Se electrocatalyst enables the selective conversion of 4-NBA to 4-aminobenzyl alcohol during the discharge process and to 4-nitrobenzoic acid during the charge process, with Faradaic efficiencies above 96%. Consequently, the 4-NBA-assisted rechargeable Zn-redox battery achieves a high power energy density of 16.13 mW cm−2 and maintains a stable yield rate of 15.92 µmol h−1 cm−2 for 4-aminobenzyl alcohol and 22.84 µmol h−1 cm−2 for 4-nitrobenzoic acid. This work presents an appealing strategy for integrating energy storage with the-whole-process chemical production, paving the way for developing multifunctional energy systems.
{"title":"A Rechargeable Zn-Redox Battery for Concurrent Electricity Generation and The-Whole-Process Chemical Production","authors":"Xiaoyang He, Shujie Xue, Xuan Liu, Dengke Xiong, Xin Xiao, Deli Wu, Jianying Wang, Qiang Xu, Zuofeng Chen","doi":"10.1002/aenm.202405473","DOIUrl":"https://doi.org/10.1002/aenm.202405473","url":null,"abstract":"The rechargeable Zn-redox battery represents a promising, efficient, and sustainable energy storage technology. Herein, a novel 4-nitrobenzyl alcohol (4-NBA)-assisted rechargeable Zn-redox battery, driven by NiSe─Cu<sub>2</sub>Se/NF bifunctional electrocatalysts is developed. The different redox activities of ─NO<sub>2</sub> and ─OH groups in 4-NBA allow redox conversion for chemical production during the whole discharge/charge process, maximizing the economic value of battery technologies. Detailed charge analyses indicate that the internal electric field within the NiSe─Cu<sub>2</sub>Se heterostructure modulates the d-band center, optimizes the adsorption/desorption strength of intermediates, and reduces the reaction energy barriers during the redox conversion of 4-NBA. This bifunctional NiSe─Cu<sub>2</sub>Se electrocatalyst enables the selective conversion of 4-NBA to 4-aminobenzyl alcohol during the discharge process and to 4-nitrobenzoic acid during the charge process, with Faradaic efficiencies above 96%. Consequently, the 4-NBA-assisted rechargeable Zn-redox battery achieves a high power energy density of 16.13 mW cm<sup>−2</sup> and maintains a stable yield rate of 15.92 µmol h<sup>−1</sup> cm<sup>−2</sup> for 4-aminobenzyl alcohol and 22.84 µmol h<sup>−1</sup> cm<sup>−2</sup> for 4-nitrobenzoic acid. This work presents an appealing strategy for integrating energy storage with the-whole-process chemical production, paving the way for developing multifunctional energy systems.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"31 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143375629","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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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