Selective CO2 electroreduction toward multicarbons (C2+) is hampered by the competing pathways at ampere-level current densities. Here, theoretical calculations reveal that the binding strength and protonation of the ∗CO intermediate are a pair of key descriptors in governing the selectivity-determining bifurcation pathway on copper (Cu) catalyst. Hence, we propose an intermediate-modulator strategy with a nonmetallic phosphorus (P)-modified Cu (P-Cu) hetero-site catalyst for ideal C2+ formation. The P site enhances charge accumulation at the neighboring Cu site, which strengthens ∗CO adsorption and active ∗H supply from H2O activation, favoring a rich-∗H-assisted-protonation (RHP) pathway toward ∗CHO formation. Subsequently, the lowest-energy-barrier ∗CO-∗CHO coupling pathway switches the predominant reaction pathway away from undesired CO and H2 to higher-value ethylene and ethanol. We report a C2+ partial current density of 1.05 A cm−2 and a Faradaic efficiency of 87.7%. Utilizing cheaper nonmetallic elements, this catalyst design principle outperforms reported outcomes with precious metal dopants.
在安培级电流密度下，二氧化碳向多碳（C2+）的选择性电还原受到竞争途径的阻碍。理论计算显示，∗CO 中间体的结合强度和质子化是铜 (Cu) 催化剂上决定选择性分叉途径的一对关键描述因子。因此，我们提出了一种中间体调节器策略，即使用非金属磷（P）修饰的铜（P-Cu）杂化位催化剂来实现理想的 C2+ 生成。P 位点增强了邻近 Cu 位点的电荷积累，从而加强了∗CO 的吸附和 H2O 活化产生的活性∗H 供应，有利于通过富∗H 辅助质子化 (RHP) 途径形成∗CHO。随后，能障最低的 ∗CO-∗CHO 偶联途径将主要反应途径从不感兴趣的 CO 和 H2 转变为价值更高的乙烯和乙醇。我们报告的 C2+ 部分电流密度为 1.05 A cm-2，法拉第效率为 87.7%。利用更廉价的非金属元素，这种催化剂的设计原理优于已报道的使用贵金属掺杂剂的结果。
{"title":"Neighboring nonmetal site as an intermediate modulator switching CO2 electroreduction pathway toward multicarbons","authors":"Li Li, Ying Zhou, Chaofan Wan, Xiaodong Li, Panzhe Qiao, Shibo Xi, Yan Fang, Xianbiao Fu, Jiexin Zhu, Shumin Wang, Xia Wang, Chengbin Xu, Zechao Zhuang, Ming Zuo, Minghui Fan, Zheng Jiang, Wenhua Zhang, Xinliang Feng, Yongfu Sun, Jinlong Yang, Yi Xie","doi":"10.1016/j.joule.2025.101926","DOIUrl":"https://doi.org/10.1016/j.joule.2025.101926","url":null,"abstract":"Selective CO<sub>2</sub> electroreduction toward multicarbons (C<sub>2+</sub>) is hampered by the competing pathways at ampere-level current densities. Here, theoretical calculations reveal that the binding strength and protonation of the ∗CO intermediate are a pair of key descriptors in governing the selectivity-determining bifurcation pathway on copper (Cu) catalyst. Hence, we propose an intermediate-modulator strategy with a nonmetallic phosphorus (P)-modified Cu (P-Cu) hetero-site catalyst for ideal C<sub>2+</sub> formation. The P site enhances charge accumulation at the neighboring Cu site, which strengthens ∗CO adsorption and active ∗H supply from H<sub>2</sub>O activation, favoring a rich-∗H-assisted-protonation (RHP) pathway toward ∗CHO formation. Subsequently, the lowest-energy-barrier ∗CO-∗CHO coupling pathway switches the predominant reaction pathway away from undesired CO and H<sub>2</sub> to higher-value ethylene and ethanol. We report a C<sub>2+</sub> partial current density of 1.05 A cm<sup>−2</sup> and a Faradaic efficiency of 87.7%. Utilizing cheaper nonmetallic elements, this catalyst design principle outperforms reported outcomes with precious metal dopants.","PeriodicalId":343,"journal":{"name":"Joule","volume":"126 1","pages":""},"PeriodicalIF":39.8,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143862362","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}
Pub Date : 2025-04-22DOI: 10.1016/j.joule.2025.101923
Channing K. Klein, Alexis Lindenfelser, Michael A. Yusov, Anukta Jain, Ryan J.R. Jones, John Gregoire, Karthish Manthiram
Artificial ammonia synthesis is vital to modern life; however, the Haber-Bosch process, by which most ammonia is synthesized, is capital and carbon intensive. Zero-valent-metal-mediated ammonia synthesis is a promising alternative but requires a metal that is both a strong reductant and forms a stable nitride. Only a small number of metals, like lithium, can satisfy these constraints. Therefore, we developed an electrochemical paradigm enabling the use of different reductants by orthogonalizing the roles of the zero-valent metal between sodium metal and a Ti active site. These components are cheaper than lithium by two orders of magnitude. Using a sodium-naphthalene-titanium cascade, we achieved a rate of 475 nmol cm−2 s−1 and a Faradaic efficiency of 24% and found that the reaction rate depends primarily on current density.
{"title":"Sodium-mediated redox cascade for electrochemical ammonia synthesis","authors":"Channing K. Klein, Alexis Lindenfelser, Michael A. Yusov, Anukta Jain, Ryan J.R. Jones, John Gregoire, Karthish Manthiram","doi":"10.1016/j.joule.2025.101923","DOIUrl":"https://doi.org/10.1016/j.joule.2025.101923","url":null,"abstract":"Artificial ammonia synthesis is vital to modern life; however, the Haber-Bosch process, by which most ammonia is synthesized, is capital and carbon intensive. Zero-valent-metal-mediated ammonia synthesis is a promising alternative but requires a metal that is both a strong reductant and forms a stable nitride. Only a small number of metals, like lithium, can satisfy these constraints. Therefore, we developed an electrochemical paradigm enabling the use of different reductants by orthogonalizing the roles of the zero-valent metal between sodium metal and a Ti active site. These components are cheaper than lithium by two orders of magnitude. Using a sodium-naphthalene-titanium cascade, we achieved a rate of 475 nmol cm<sup>−2</sup> s<sup>−1</sup> and a Faradaic efficiency of 24% and found that the reaction rate depends primarily on current density.","PeriodicalId":343,"journal":{"name":"Joule","volume":"12 1","pages":""},"PeriodicalIF":39.8,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143858173","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}
Pub Date : 2025-04-18DOI: 10.1016/j.joule.2025.101927
Sungmin Park, Seongwon Yoon, Hyungju Ahn, Hyeonggeun Yu, Eul-Yong Shin, Kangsik Cho, Yoon Hee Jang, Yongseok Jun, Hae Jung Son
Dielectric material in bulk-heterojunctions can play critical roles in exciton polarization and morphology control. We develop carvone (CV) dielectric additive to prepare high-efficiency, large-area organic photovoltaics (OPVs). CV forms a complex with L8-BO, which enhances forming uniform crystallites of acceptors as well as exciton dissociation in D18:N3:L8-BO blend. Furthermore, strong inward Marangoni flows induced by CV addition during blade coating enable the evolution of homogeneous morphology over large areas, irrespective of the surface energy of the electron-transporting layer. As a result, OPVs exhibited improved performances and, in particular, the device using binary D18:PM6 donors achieved efficiency of 17.44% for an active area of 1 cm2 and the corresponding module showed 16.27% efficiency. This is among the highest OPV module efficiency achieved, with active areas above 20 cm2. Importantly, it is demonstrated that CV addition is effective for reproducible preparation of the optimal blend morphology in ambient air with relative humidity from 10% to 70%.
{"title":"Dielectric additive enables humidity-independent preparation of blend morphology for high-performance, large-area organic photovoltaics","authors":"Sungmin Park, Seongwon Yoon, Hyungju Ahn, Hyeonggeun Yu, Eul-Yong Shin, Kangsik Cho, Yoon Hee Jang, Yongseok Jun, Hae Jung Son","doi":"10.1016/j.joule.2025.101927","DOIUrl":"https://doi.org/10.1016/j.joule.2025.101927","url":null,"abstract":"Dielectric material in bulk-heterojunctions can play critical roles in exciton polarization and morphology control. We develop carvone (CV) dielectric additive to prepare high-efficiency, large-area organic photovoltaics (OPVs). CV forms a complex with L8-BO, which enhances forming uniform crystallites of acceptors as well as exciton dissociation in D18:N3:L8-BO blend. Furthermore, strong inward Marangoni flows induced by CV addition during blade coating enable the evolution of homogeneous morphology over large areas, irrespective of the surface energy of the electron-transporting layer. As a result, OPVs exhibited improved performances and, in particular, the device using binary D18:PM6 donors achieved efficiency of 17.44% for an active area of 1 cm<sup>2</sup> and the corresponding module showed 16.27% efficiency. This is among the highest OPV module efficiency achieved, with active areas above 20 cm<sup>2</sup>. Importantly, it is demonstrated that CV addition is effective for reproducible preparation of the optimal blend morphology in ambient air with relative humidity from 10% to 70%.","PeriodicalId":343,"journal":{"name":"Joule","volume":"381 1","pages":""},"PeriodicalIF":39.8,"publicationDate":"2025-04-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143846529","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}
Pub Date : 2025-04-16DOI: 10.1016/j.joule.2025.101851
Ming Zhang (张明) , Lei Zhu , Jun Yan , Xiaonan Xue , Zaiyu Wang , Flurin Eisner , Guanqing Zhou , Rui Zeng , Lixuan Kan , Liang Wu , Wenkai Zhong , Anyang Zhang , Fei Han , Jingnan Song , Nicolai Hartmann , Zichun Zhou , Hao Jing , Haiming Zhu , Shengjie Xu (许胜杰) , Jenny Nelson , Feng Liu (刘烽)
The lack of simultaneous high efficiency and long-term stability in organic photovoltaics (OPVs) poses a major challenge to commercialization. Here, we introduce a high-entropy (HE) methodology by both physical blending and chemical synthesis, where multiple components are mixed to improve system entropy. Our findings show that physically blended HE blends maintained strong π–π interactions due to acceptors’ identical backbones. The different halogens or alkyl chains reduced structure order and fostered an optimal mixture, where a redistribution of the conduction-band density of states was found, leading to a higher effective band gap, reduced non-radiative recombination, and elevated open-circuit voltage. This HE design rule was then extended to chemical synthesis to make HE materials, which yielded a maximum power conversion efficiency of 20.6% (20.3% ± 0.2%, certified as 20.0%) in OPV devices. Moreover, both operational and thermal stability were improved, measured in conventional encapsulated devices under continuous illumination.
{"title":"Efficient and stable high-entropy organic photovoltaics","authors":"Ming Zhang (张明) , Lei Zhu , Jun Yan , Xiaonan Xue , Zaiyu Wang , Flurin Eisner , Guanqing Zhou , Rui Zeng , Lixuan Kan , Liang Wu , Wenkai Zhong , Anyang Zhang , Fei Han , Jingnan Song , Nicolai Hartmann , Zichun Zhou , Hao Jing , Haiming Zhu , Shengjie Xu (许胜杰) , Jenny Nelson , Feng Liu (刘烽)","doi":"10.1016/j.joule.2025.101851","DOIUrl":"10.1016/j.joule.2025.101851","url":null,"abstract":"<div><div>The lack of simultaneous high efficiency and long-term stability in organic photovoltaics (OPVs) poses a major challenge to commercialization. Here, we introduce a high-entropy (HE) methodology by both physical blending and chemical synthesis, where multiple components are mixed to improve system entropy. Our findings show that physically blended HE blends maintained strong π–π interactions due to acceptors’ identical backbones. The different halogens or alkyl chains reduced structure order and fostered an optimal mixture, where a redistribution of the conduction-band density of states was found, leading to a higher effective band gap, reduced non-radiative recombination, and elevated open-circuit voltage. This HE design rule was then extended to chemical synthesis to make HE materials, which yielded a maximum power conversion efficiency of 20.6% (20.3% ± 0.2%, certified as 20.0%) in OPV devices. Moreover, both operational and thermal stability were improved, measured in conventional encapsulated devices under continuous illumination.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 4","pages":"Article 101851"},"PeriodicalIF":38.6,"publicationDate":"2025-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143539141","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}
Pub Date : 2025-04-16DOI: 10.1016/j.joule.2025.101825
Mingyu Li , Jun Yan , Afei Zhang , Xinzhao Zhao , Xuke Yang , Shuwen Yan , Ning Ma , Tianjun Ma , Dingfu Luo , Zhenhua Chen , Luying Li , Xiong Li , Chao Chen , Haisheng Song , Jiang Tang
The power conversion efficiency of all-perovskite tandem solar cells (TSCs) suffers from inferior film quality and the susceptible fabrication processes of lead-tin narrow band-gap (Pb-Sn NBG) perovskite subcells. Herein, we developed a robust vacuum-driven precrystallization (VDP) strategy for high-quality Pb-Sn NBG perovskite films. Compared with traditional anti-solvent methods, the present precrystallization step could significantly retard the perovskite crystallization process by mild vacuum pumping. The above evolution process was quantitatively studied for the perovskite intermediate phase (PIP). The slow solvent extraction of the VDP strategy promotes a low surface energy of (100) plane-oriented precrystallization and provides sufficient time for grain ripening. The obtained Pb-Sn perovskite presented overall texture homogeneity and high crystallinity. The resulting all-perovskite TSCs yielded a top certified efficiency of 28.87% (28.09%) under reverse (forward) scan. Our VDP strategy promises efficient perovskite TSCs and contributes a key step toward robust and scalable photovoltaic technology.
{"title":"Vacuum-driven precrystallization enables efficient all-perovskite tandem solar cells","authors":"Mingyu Li , Jun Yan , Afei Zhang , Xinzhao Zhao , Xuke Yang , Shuwen Yan , Ning Ma , Tianjun Ma , Dingfu Luo , Zhenhua Chen , Luying Li , Xiong Li , Chao Chen , Haisheng Song , Jiang Tang","doi":"10.1016/j.joule.2025.101825","DOIUrl":"10.1016/j.joule.2025.101825","url":null,"abstract":"<div><div>The power conversion efficiency of all-perovskite tandem solar cells (TSCs) suffers from inferior film quality and the susceptible fabrication processes of lead-tin narrow band-gap (Pb-Sn NBG) perovskite subcells. Herein, we developed a robust vacuum-driven precrystallization (VDP) strategy for high-quality Pb-Sn NBG perovskite films. Compared with traditional anti-solvent methods, the present precrystallization step could significantly retard the perovskite crystallization process by mild vacuum pumping. The above evolution process was quantitatively studied for the perovskite intermediate phase (PIP). The slow solvent extraction of the VDP strategy promotes a low surface energy of (100) plane-oriented precrystallization and provides sufficient time for grain ripening. The obtained Pb-Sn perovskite presented overall texture homogeneity and high crystallinity. The resulting all-perovskite TSCs yielded a top certified efficiency of 28.87% (28.09%) under reverse (forward) scan. Our VDP strategy promises efficient perovskite TSCs and contributes a key step toward robust and scalable photovoltaic technology.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 4","pages":"Article 101825"},"PeriodicalIF":38.6,"publicationDate":"2025-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143083875","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}
Pub Date : 2025-04-16DOI: 10.1016/j.joule.2025.101874
Guanjie Li , Dengpan Dong , Dmitry Bedrov , Qinqin Cai , Haojun Wu , Zixing Wang , Jilei Liu , Kang Xu , Lidan Xing , Weishan Li
The electrode/electrolyte interphases in advanced batteries are critical for their performance, influencing the reversibility and rate capability of cell reactions. Although much research has focused on the electrolyte side, our study reveals the significant impact of the electrode’s interlayer distance on interphasial chemistry. We discovered that smaller interlayer distances in graphitic anodes lead to higher sensitivity to co-intercalation of Li+ and solvents, resulting in LiF-poor interphases that reduce stability. Conversely, larger interlayer distances allow anion-rich solvation structures, resulting in LiF-rich interphases and facilitating reversible intercalation/deintercalation reactions. This correlation between interlayer distance and interphasial chemistry offers new strategies for designing next-generation battery electrolytes and electrodes, moving beyond electrolyte engineering to include electrode structural considerations. Our findings are universally applicable across diverse electrolyte systems, providing a robust framework for optimizing battery performance.
{"title":"Correlating electrode nano-confinement to interphase chemistry","authors":"Guanjie Li , Dengpan Dong , Dmitry Bedrov , Qinqin Cai , Haojun Wu , Zixing Wang , Jilei Liu , Kang Xu , Lidan Xing , Weishan Li","doi":"10.1016/j.joule.2025.101874","DOIUrl":"10.1016/j.joule.2025.101874","url":null,"abstract":"<div><div>The electrode/electrolyte interphases in advanced batteries are critical for their performance, influencing the reversibility and rate capability of cell reactions. Although much research has focused on the electrolyte side, our study reveals the significant impact of the electrode’s interlayer distance on interphasial chemistry. We discovered that smaller interlayer distances in graphitic anodes lead to higher sensitivity to co-intercalation of Li<sup>+</sup> and solvents, resulting in LiF-poor interphases that reduce stability. Conversely, larger interlayer distances allow anion-rich solvation structures, resulting in LiF-rich interphases and facilitating reversible intercalation/deintercalation reactions. This correlation between interlayer distance and interphasial chemistry offers new strategies for designing next-generation battery electrolytes and electrodes, moving beyond electrolyte engineering to include electrode structural considerations. Our findings are universally applicable across diverse electrolyte systems, providing a robust framework for optimizing battery performance.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 4","pages":"Article 101874"},"PeriodicalIF":38.6,"publicationDate":"2025-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143618887","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}
Pub Date : 2025-04-16DOI: 10.1016/j.joule.2025.101917
Hongrun Jin , Dongyuan Zhao , Dongliang Chao
Quantitative descriptors in electrolyte engineering facilitate the rational design of Zn-based aqueous batteries (ZABs). In a recent issue of Joule, Wang et al. proposed comprehensive criteria for selecting organic molecules for ZABs electrolytes. This preview summarizes the key criteria in electrolyte engineering and provides insights into the development of ZABs.
{"title":"Quantitative electrolyte engineering for Zn-based aqueous batteries","authors":"Hongrun Jin , Dongyuan Zhao , Dongliang Chao","doi":"10.1016/j.joule.2025.101917","DOIUrl":"10.1016/j.joule.2025.101917","url":null,"abstract":"<div><div>Quantitative descriptors in electrolyte engineering facilitate the rational design of Zn-based aqueous batteries (ZABs). In a recent issue of <em>Joule</em>, Wang et al. proposed comprehensive criteria for selecting organic molecules for ZABs electrolytes. This preview summarizes the key criteria in electrolyte engineering and provides insights into the development of ZABs.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 4","pages":"Article 101917"},"PeriodicalIF":38.6,"publicationDate":"2025-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143834050","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}
Pub Date : 2025-04-16DOI: 10.1016/j.joule.2025.101854
Sichen Duan , Xin Bao , Jiawei Huang , Rongpei Shi , Linfeng Fei , Wenhua Xue , Honghao Yao , Xiaofang Li , Jian Wang , Xingjun Liu , Jun Mao , Feng Cao , Yumei Wang , Qian Zhang
Spinodal decomposition typically manifests in partially miscible solid solutions in relevant phase diagrams as primarily dictated by the underlying thermodynamics, which is viewed as a powerful means for enhancing thermoelectric performance. Yet, the incomplete ternary phase diagrams of thermoelectric materials pose a challenge for microstructure design via spinodal decomposition. In addition, experimental investigation of microstructure evolution upon spinodal decomposition in thermoelectric alloys is rare, and its influence on electron and phonon transport remains largely unexplored. Herein, we constructed the (Ti, Zr, Hf)NiSn phase diagram experimentally, revealing a miscibility gap within 973–1,273 K. Spinodal decomposition with anisotropic composition modulation was observed in Ti0.5Zr0.25Hf0.25NiSn0.99Sb0.01 by in situ transmission electron microscopy. The phase-field simulation further elucidates the microstructure evolution upon spinodal decomposition and provides insights into the generation of dislocations during further heat treatment. The annealing process not only induces dense dislocation arrays formed by spinodal evolution but also homogenizes the multiphase to facilitate electron transport. Consequently, a record-high average zT of ∼1.1 between 300 and 973 K has been realized in n-type Ti0.5Zr0.25Hf0.25NiSn0.99Sb0.01. Importantly, the half-Heusler module achieves a maximum conversion efficiency of ∼12% and an output power density of ∼3.7 W cm−2 at a temperature difference of 653 K. This “double-high” result outperforms all of the current devices. Our results highlight spinodal decomposition as an effective avenue to advance materials for highly efficient thermoelectric power generation.
{"title":"Spinodal decomposition promoting high thermoelectric performance in half-Heusler","authors":"Sichen Duan , Xin Bao , Jiawei Huang , Rongpei Shi , Linfeng Fei , Wenhua Xue , Honghao Yao , Xiaofang Li , Jian Wang , Xingjun Liu , Jun Mao , Feng Cao , Yumei Wang , Qian Zhang","doi":"10.1016/j.joule.2025.101854","DOIUrl":"10.1016/j.joule.2025.101854","url":null,"abstract":"<div><div>Spinodal decomposition typically manifests in partially miscible solid solutions in relevant phase diagrams as primarily dictated by the underlying thermodynamics, which is viewed as a powerful means for enhancing thermoelectric performance. Yet, the incomplete ternary phase diagrams of thermoelectric materials pose a challenge for microstructure design via spinodal decomposition. In addition, experimental investigation of microstructure evolution upon spinodal decomposition in thermoelectric alloys is rare, and its influence on electron and phonon transport remains largely unexplored. Herein, we constructed the (Ti, Zr, Hf)NiSn phase diagram experimentally, revealing a miscibility gap within 973–1,273 K. Spinodal decomposition with anisotropic composition modulation was observed in Ti<sub>0.5</sub>Zr<sub>0.25</sub>Hf<sub>0.25</sub>NiSn<sub>0.99</sub>Sb<sub>0.01</sub> by <em>in situ</em> transmission electron microscopy. The phase-field simulation further elucidates the microstructure evolution upon spinodal decomposition and provides insights into the generation of dislocations during further heat treatment. The annealing process not only induces dense dislocation arrays formed by spinodal evolution but also homogenizes the multiphase to facilitate electron transport. Consequently, a record-high average <em>zT</em> of ∼1.1 between 300 and 973 K has been realized in n-type Ti<sub>0.5</sub>Zr<sub>0.25</sub>Hf<sub>0.25</sub>NiSn<sub>0.99</sub>Sb<sub>0.01</sub>. Importantly, the half-Heusler module achieves a maximum conversion efficiency of ∼12% and an output power density of ∼3.7 W cm<sup>−2</sup> at a temperature difference of 653 K. This “double-high” result outperforms all of the current devices. Our results highlight spinodal decomposition as an effective avenue to advance materials for highly efficient thermoelectric power generation.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 4","pages":"Article 101854"},"PeriodicalIF":38.6,"publicationDate":"2025-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143560950","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}
Pub Date : 2025-04-16DOI: 10.1016/j.joule.2025.101887
Mengqi Liu , Shenghao Jin , Chenglong Zhou , Boxiang Wang , Changying Zhao , Cheng-Wei Qiu
<div><div>Mengqi Liu received her bachelor’s degree in energy and power engineering from Shandong University in 2016 and a joint PhD degree in engineering thermophysics from Shanghai Jiao Tong University (SJTU) and National University of Singapore (NUS) in 2022. Now, she is a postdoctoral researcher at SJTU and a visiting scholar at NUS. Her research interests include micro/nanoscale thermal radiation, nonreciprocal thermal photonics, topological properties in thermal photoncis, metamaterials energy devices, etc.</div><div>Shenghao Jin obtained his bachelor’s degree at the School of Energy and Power Engineering at Dalian University of Technology, China. He is currently a PhD student in the Institute of Engineering Thermophysics at SJTU, China. His research interests include the design of colorful radiative cooling devices, smart windows, electrochromic display, and efficient dynamic spectrum engineering.</div><div>Chenglong Zhou obtained his bachelor’s degree in energy and power engineering from Harbin Engineering University, a master’s degree in engineering thermophysics from Harbin Institute of Technology, and a PhD from Harbin Institute of Technology. After that, he joined the Department of Energy Science and Engineering, Harbin Institute of Technology, in 2024, where he is currently working as an associate researcher. He works in the near-field radiative heat transfer, aiming to address the constraints imposed by the blackbody radiation limit and the challenges in precise regulation of radiative energy utilization within novel energy systems.</div><div>Boxiang Wang received a BS degree from Huazhong University of Science and Technology in 2012 and then a PhD from SJTU in 2018. Then he worked successively as a postdoctoral researcher (2018–2021), an assistant professor (2021–2022), and then an associate professor (2022–2024) at the same university. After that, he joined Shanghai Institute of Microsystem and Information Technology (SIMIT), Chinese Academy of Sciences, as a young professor and the principal investigator of SIMIT Thermal Radiation Group. His research interests include nanoscale thermal radiation, nanophotonics, micro-electro-mechanical system (MEMS) sensors, smart windows and radiative cooling.</div><div>Changying Zhao is the chair professor and the director of the Institute of Engineering Thermophysics of SJTU. His research covers micro/nanoscale thermal radiation and metamaterial energy devices, advanced thermal energy storage and hydrogen storage, and heat transfer in porous media. He has published over 300 papers in peer-reviewed high-quality journals with over 20,000 citations in total. His contributions have been recognized through prestigious awards, including a 2023 William Begell Medal and 2024 Prominent Research Award. He is the editor-in-chief of <em>Carbon Neutrality</em>, an associate editor of <em>Thermal Science and Engineering Progress</em>, and an editorial board member of several other international journals.</d
{"title":"An inconvenient truth of thermal nonreciprocity’s impact on radiative cooling efficiency","authors":"Mengqi Liu , Shenghao Jin , Chenglong Zhou , Boxiang Wang , Changying Zhao , Cheng-Wei Qiu","doi":"10.1016/j.joule.2025.101887","DOIUrl":"10.1016/j.joule.2025.101887","url":null,"abstract":"<div><div>Mengqi Liu received her bachelor’s degree in energy and power engineering from Shandong University in 2016 and a joint PhD degree in engineering thermophysics from Shanghai Jiao Tong University (SJTU) and National University of Singapore (NUS) in 2022. Now, she is a postdoctoral researcher at SJTU and a visiting scholar at NUS. Her research interests include micro/nanoscale thermal radiation, nonreciprocal thermal photonics, topological properties in thermal photoncis, metamaterials energy devices, etc.</div><div>Shenghao Jin obtained his bachelor’s degree at the School of Energy and Power Engineering at Dalian University of Technology, China. He is currently a PhD student in the Institute of Engineering Thermophysics at SJTU, China. His research interests include the design of colorful radiative cooling devices, smart windows, electrochromic display, and efficient dynamic spectrum engineering.</div><div>Chenglong Zhou obtained his bachelor’s degree in energy and power engineering from Harbin Engineering University, a master’s degree in engineering thermophysics from Harbin Institute of Technology, and a PhD from Harbin Institute of Technology. After that, he joined the Department of Energy Science and Engineering, Harbin Institute of Technology, in 2024, where he is currently working as an associate researcher. He works in the near-field radiative heat transfer, aiming to address the constraints imposed by the blackbody radiation limit and the challenges in precise regulation of radiative energy utilization within novel energy systems.</div><div>Boxiang Wang received a BS degree from Huazhong University of Science and Technology in 2012 and then a PhD from SJTU in 2018. Then he worked successively as a postdoctoral researcher (2018–2021), an assistant professor (2021–2022), and then an associate professor (2022–2024) at the same university. After that, he joined Shanghai Institute of Microsystem and Information Technology (SIMIT), Chinese Academy of Sciences, as a young professor and the principal investigator of SIMIT Thermal Radiation Group. His research interests include nanoscale thermal radiation, nanophotonics, micro-electro-mechanical system (MEMS) sensors, smart windows and radiative cooling.</div><div>Changying Zhao is the chair professor and the director of the Institute of Engineering Thermophysics of SJTU. His research covers micro/nanoscale thermal radiation and metamaterial energy devices, advanced thermal energy storage and hydrogen storage, and heat transfer in porous media. He has published over 300 papers in peer-reviewed high-quality journals with over 20,000 citations in total. His contributions have been recognized through prestigious awards, including a 2023 William Begell Medal and 2024 Prominent Research Award. He is the editor-in-chief of <em>Carbon Neutrality</em>, an associate editor of <em>Thermal Science and Engineering Progress</em>, and an editorial board member of several other international journals.</d","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 4","pages":"Article 101887"},"PeriodicalIF":38.6,"publicationDate":"2025-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143767050","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}
Pub Date : 2025-04-16DOI: 10.1016/j.joule.2025.101918
Hai Wang , Feng-Shou Xiao
In recent issues of Nature and Science, Ma and colleagues demonstrate novel catalytic strategies for hydrogen production from alcohol reforming over γ-Mo2N and α-MoC supported metal catalysts, achieving excellent performance, even at near-zero carbon dioxide emission. These studies emphasize the importance of γ-Mo2N and α-MoC for sustainable hydrogen production.
{"title":"Active support of γ-Mo2N and α-MoC for sustainable hydrogen production","authors":"Hai Wang , Feng-Shou Xiao","doi":"10.1016/j.joule.2025.101918","DOIUrl":"10.1016/j.joule.2025.101918","url":null,"abstract":"<div><div>In recent issues of <em>Nature</em> and <em>Science</em>, Ma and colleagues demonstrate novel catalytic strategies for hydrogen production from alcohol reforming over γ-Mo<sub>2</sub>N and α-MoC supported metal catalysts, achieving excellent performance, even at near-zero carbon dioxide emission. These studies emphasize the importance of γ-Mo<sub>2</sub>N and α-MoC for sustainable hydrogen production.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 4","pages":"Article 101918"},"PeriodicalIF":38.6,"publicationDate":"2025-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143833338","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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