Materials Today Physics最新文献

{"title":"Ce doping induces lattice expansion of cobalt oxide electrocatalyst to achieve efficient proton exchange membrane water electrolysis","authors":"Zhi Wang ,&nbsp;Jinpeng Li ,&nbsp;Chengdeng Wang ,&nbsp;Jiashuai Wang ,&nbsp;Xiangrui Chen ,&nbsp;Jun Wu ,&nbsp;Zhiming Bai ,&nbsp;Yan Gao ,&nbsp;Li Chen ,&nbsp;Xiaoqin Yan","doi":"10.1016/j.mtphys.2024.101641","DOIUrl":"10.1016/j.mtphys.2024.101641","url":null,"abstract":"<div><div>The development of non-precious metal anode catalysts with high performance and low cost for proton exchange membrane (PEM) water electrolysis presents a significant challenge. This work successfully synthesized a bimetallic-doped cobalt-based oxide titanium diboride composite structure catalyst (Ce-Mn-Co₃O₄/TiB₂) by combining hydrothermal methods with heat treatment processes. Ce doping induces surface oxygen vacancies of Co₃O₄ to optimize adsorption energy, while Mn stabilizes lattice oxygen and impedes the dissolution of metal ions. Theoretical simulations support the experimental results, highlighting the strain effect of Ce doping on the Co₃O₄-TiB₂ interface, promoting further charge redistribution, and enhancing catalyst conductivity. Ce-Mn-Co₃O₄/TiB₂ exhibits a low oxygen evolution overpotential (389 mV @10 mA/cm²). Upon assembly into a PEM electrolytic cell, it achieves a current density of 250 mA/cm² at 1.63 V and demonstrates stable operation for nearly 25 h. This research provides novel ideas and methodologies for developing non-precious metal OER electrocatalysts suitable for PEM electrolysis.</div></div>","PeriodicalId":18253,"journal":{"name":"Materials Today Physics","volume":"51 ","pages":"Article 101641"},"PeriodicalIF":10.0,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142908416","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}

{"title":"Innovative dual-band energy-efficient smart windows using VO2(M)-Based Fabry-Pérot structures for solar and radiative cooling modulation","authors":"Joonho Keum ,&nbsp;Jun Choi ,&nbsp;Sujin Kim ,&nbsp;Guyoung Kang ,&nbsp;Byuonghong Lee ,&nbsp;Min Jae Lee ,&nbsp;Woochul Kim","doi":"10.1016/j.mtphys.2025.101665","DOIUrl":"10.1016/j.mtphys.2025.101665","url":null,"abstract":"<div><div>Thermochromic windows have been studied as a promising solution for energy-efficiency with the dynamical adjustment of solar heating in response to temperature. Recent advancements in the field have introduced simultaneous multiband modulation, incorporating radiative cooling in the longwave infrared range. In this work, we present VO₂(M)/TiO₂(A)/ITO multilayer-coated glass (referred to as VTI) as a scalable and effective smart window that modulates both solar transmission and radiative cooling concurrently. As a semitransparent window in the solar spectrum, the VTI coating achieves nearly 100 % visual clarity, 38.5 % visible transparency, and 8.5 % modulation of solar transmittance. In the longwave infrared region, the VTI multilayer demonstrates an exceptional broadband emissivity shift of up to 42.5 %, made possible by an innovative Fabry-Pérot (F-P) cavity composed of absorbing metal oxides. This high degree of emissivity modulation is maintained across a wide range of spacer thicknesses, from 100 to 500 nm, as confirmed by both experimental data and simulations. The modulation mechanism of the F-P cavity which use ultrathin spacer (<em>λ</em>/140 ∼ <em>λ</em>/16) at its resonant absorption range is explained through incremental phasor analysis by the transfer-matrix method. Additionally, the scalability and practicality of the VTI film are supported by its three-layer composition and the room-temperature reactive magnetron sputtering deposition process. These results suggest that the design principles presented here could inspire further innovations in broadband longwave infrared emissivity modulation, utilizing ultrathin F-P cavities composed of semitransparent metal oxides.</div></div>","PeriodicalId":18253,"journal":{"name":"Materials Today Physics","volume":"52 ","pages":"Article 101665"},"PeriodicalIF":10.0,"publicationDate":"2025-01-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143071791","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}

{"title":"Optimized pyramidal honeycomb PEEK/CF composites metastructure through 3D printing for broadband electromagnetic wave absorption","authors":"Ximing Zhang ,&nbsp;Guoke Wei ,&nbsp;Xinghan Huang ,&nbsp;Hang Zhang ,&nbsp;Xingyu Hao ,&nbsp;Shujuan Tan ,&nbsp;Kui Liu ,&nbsp;Guangbin Ji","doi":"10.1016/j.mtphys.2024.101620","DOIUrl":"10.1016/j.mtphys.2024.101620","url":null,"abstract":"<div><div>This study presents a novel pyramidal honeycomb metastructure, which integrates the geometric advantages of honeycomb and pyramid designs to achieve highly effective electromagnetic wave (EMW) absorption with reduced thickness. The pyramidal honeycomb metastructure capitalizes on the angle insensitivity characteristics of pyramidal geometries while leveraging the weight reduction benefits inherent in honeycomb designs. This metastructure is fabricated using an additive manufacturing (AM) process, specifically employing PEEK/CF composite through the fused deposition modeling (FDM) method, followed by a spraying process. The dimensions of the pyramidal honeycomb metastructure were optimized using simulation process, and its EMW absorption mechanism was thoroughly analyzed. The effective absorption bandwidth (EAB) of the composite metastructure nearly spans the Ku, K, and Ka bands at thin thicknesses, maintaining high performance even at incidence angles up to 45°. This research provides a valuable approach for aerospace applications, expanding the potential of 3D printing technologies in multi-scenario EMW absorption.</div></div>","PeriodicalId":18253,"journal":{"name":"Materials Today Physics","volume":"50 ","pages":"Article 101620"},"PeriodicalIF":10.0,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142793226","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}

{"title":"Large magnetocaloric effect near liquid hydrogen temperatures in Er1-xTmxGa materials","authors":"Dingsong Wang ,&nbsp;Xinqi Zheng ,&nbsp;Lunhua He ,&nbsp;Hui Wu ,&nbsp;Yawei Gao ,&nbsp;Guyue Wang ,&nbsp;Hao Liu ,&nbsp;Shanshan Zhen ,&nbsp;Yang Pan ,&nbsp;Zixiao Zhang ,&nbsp;Guangrui Zhang ,&nbsp;Anxu Ma ,&nbsp;Zhe Chen ,&nbsp;Lei Xi ,&nbsp;Jiawang Xu ,&nbsp;Shouguo Wang ,&nbsp;Baogen Shen","doi":"10.1016/j.mtphys.2024.101609","DOIUrl":"10.1016/j.mtphys.2024.101609","url":null,"abstract":"<div><div>Low-temperature magnetocaloric materials are of great importance for potential applications of gas liquefaction such as nitrogen, hydrogen and helium for their low liquidation temperatures (∼4 K for helium, ∼20 K for hydrogen and ∼77 K for nitrogen respectively), of which the working temperature, the maximal magnetic entropy change (<em>(-ΔS</em>_<em>M</em><em>)</em>_<em>max</em>), the maximal adiabatic temperature change (<em>(ΔT</em>_<em>ad</em><em>)</em>_<em>max</em>), and the temperature average entropy change (<em>TEC</em>) are the key assessment parameters. Herein, we designed and synthesized Er_1-xTm_xGa series compounds based on the optimization of the spin quantum number (<em>Spin</em>) with their magnetic ordering temperature successfully adjusted from 31.0 K to 15.0 K, which covers the liquid hydrogen temperature range. Particularly, Er_0.8Tm_0.2Ga shows outstanding (-ΔS_M)_max, <em>TEC</em>(20), and <em>(ΔT</em>_<em>ad</em><em>)</em>_<em>max</em> values of 13.6 J/kg K, 10.1 J/kg K, and 4.3 K under the field change of 0–2 T, respectively, which are increased by 32.0 %, 36.4 %, and 48.2 % compared with the parent ErGa compound. It should be noted that the refrigerant capacity (RC) of Er_0.8Tm_0.2Ga is not only larger than ErGa but also larger than TmGa. Furthermore, neutron powder diffraction (NPD) was employed on Er_0.8Tm_0.2Ga to reveal the physical mechanism of its enhanced magnetocaloric effect (MCE). It is found that for Er_0.8Tm_0.2Ga the more pronounced order-to-disorder transition than the spin reorientation (SR) transition, the characteristic second order phase transition, and the existence of the short-range magnetic ordering above the magnetic ordering temperature should be jointly responsible for its large magnetocaloric effect.</div></div>","PeriodicalId":18253,"journal":{"name":"Materials Today Physics","volume":"50 ","pages":"Article 101609"},"PeriodicalIF":10.0,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142735518","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}

{"title":"Rare earth stannates: A new high-performance wave-transparent material investigated through theoretical and experimental approaches","authors":"Shuping Wen,&nbsp;Zhilin Chen,&nbsp;Zhilin Tian,&nbsp;Liya Zheng,&nbsp;Bin Li","doi":"10.1016/j.mtphys.2024.101622","DOIUrl":"10.1016/j.mtphys.2024.101622","url":null,"abstract":"<div><div>Wave-transparent materials are widely used as integrated structural-functional materials in various aircraft communication systems. However, the lack of high-performance wave-transparent materials has impeded the advancement of hypersonic aircraft. Consequently, the search for novel high-performance wave-transparent materials has become a critical challenge. This study investigates the dielectric, mechanical, and thermal properties of RE₂Sn₂O₇ (RE = La, Nd, Sm, Eu, Gd, Tb, Dy, Er, and Lu) using both theoretical predictions and experimental measurements to evaluate their suitability as wave-transparent materials. Preliminary first-principles calculations predict exceptional mechanical properties for RE₂Sn₂O₇. These predictions are confirmed experimentally, with synthesized RE₂Sn₂O₇ samples exhibiting Young's modulus exceeding 200 GPa and hardness greater than 10 GPa. Additionally, they also present low dielectric constants (∼8) and dielectric loss tangent values below 0.01 with the dielectric constant unaffected by RE species, while the dielectric loss tangent value decreases as the RE³⁺ ionic radius decreases. Their thermal expansion coefficients range between of 8 × 10⁻⁶ K⁻¹ and 10 × 10⁻⁶ K⁻¹, while thermal conductivities can be as low as 2 W m⁻¹ K⁻¹. The relationship between RE³⁺ ionic radius and intrinsic properties is elucidated, revealing that a smaller ionic radius reduces dielectric loss tangent value while enhancing Young's modulus, hardness, and thermal expansion coefficient. These results provide valuable theoretical guidance for design of high-performance wave-transparent materials.</div></div>","PeriodicalId":18253,"journal":{"name":"Materials Today Physics","volume":"50 ","pages":"Article 101622"},"PeriodicalIF":10.0,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142797752","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}

{"title":"Hetero-structured construction of RGO nanosheets decorated by flower-like MoS2 toward the regulation of electromagnetic wave absorption performance","authors":"Zhengzheng Guo ,&nbsp;Ze Zong ,&nbsp;Yanyan Cao ,&nbsp;Yidan Zhao ,&nbsp;Fuqiang Wang ,&nbsp;Peien Luo ,&nbsp;Shanhui Liu ,&nbsp;Fang Ren ,&nbsp;Penggang Ren","doi":"10.1016/j.mtphys.2024.101631","DOIUrl":"10.1016/j.mtphys.2024.101631","url":null,"abstract":"<div><div>Exploring high-efficiency graphene-based electromagnetic wave (EMW) absorption materials is urgently required owing to the increasingly severe electromagnetic radiation pollution. However, the serious impedance mismatching caused by the superior conductivity of graphene and finite attenuation mechanism constrain its development. Herein, MoS₂@RGO with plentiful heterointerfaces are fabricated by a facile solvothermal strategy to realize outstanding EMW absorption. The incorporation of MoS₂ could not only effectively reduce the conductivity of RGO to alleviate the impedance mismatching issue, but also greatly enrich the loss mechanisms. In addition, the construction of flower-like MoS₂ assembled by MoS₂ could greatly prolong the transmission path of EMW through multiple reflection and scattering. The improved impedance matching and multiple dissipation mechanisms jointly endow the developed materials with brilliant EMW absorption performance. The prepared MoS₂@RGO with a 1:1 ratio of MoS₂ to RGO (MR3) at a low filler loading of 20 wt% achieves the minimum reflection loss of −69.6 dB at the frequency of 8.46 GHz under a low thickness of 2.77 mm and a broad effective absorption bandwidth of 4.36 GHz (from 11.00 to 15.36 GHz). Notably, the effectiveness of the resultant MR composites used as actual absorbers is strongly verified by the radar cross section simulation. This work opens up new possibilities for constructing hetero-structured graphene-based composites with rich heterointerfaces toward excellent electromagnetic protection.</div></div>","PeriodicalId":18253,"journal":{"name":"Materials Today Physics","volume":"50 ","pages":"Article 101631"},"PeriodicalIF":10.0,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142849493","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}

{"title":"Heteroatom-doping effects on high-temperature infrared emission of (LaPr)2Ce2O7 ceramics","authors":"Guang-Yang Xin ,&nbsp;Xieeryazidan Aday ,&nbsp;Cheng-Yu He ,&nbsp;Bao-Hua Liu ,&nbsp;Guo-Yu Ren ,&nbsp;Hui-Xia Guo ,&nbsp;Xiang-Hu Gao","doi":"10.1016/j.mtphys.2024.101615","DOIUrl":"10.1016/j.mtphys.2024.101615","url":null,"abstract":"<div><div>Manipulating thermal radiation through electromagnetic waves while maximizing heat transfer efficiency is critical for energy conservation and thermal protection in high-temperature environments. In this study, a series of heteroatom-doped (LaPr)₂Ce₂O₇ ceramics are synthesized, with a defect fluorite structure, exhibiting differential infrared radiation properties over a broad spectrum. In particular, doping with low-valence transition metals (Cu and Co) introduces impurity levels and oxygen vacancies, effectively reducing the intrinsic bandgap and increasing emissivity at wavelengths below 6 μm. Meanwhile, the mismatched properties in mass and ionic radius between the dopants and host atoms increase the asymmetry of the lattice structure, which is beneficial for long-wavelength emissivity (&gt;6 μm). The infrared emissivity of (LaPrCu)₂Ce₂O₇ reaches 0.870 across a broad wavelength range from 0.78 μm to 16 μm, surpassing that of pristine (LaPr)₂Ce₂O₇. This enhancement is attributed to the effective collaboration of impurity absorption, free carrier absorption, and lattice absorption. More importantly, the achieved near black-body thermal emissivity at 1300 °C is suitable for applications in high-temperature thermal radiation. In contrast, the introduction of rare-earth elements (Gd and Ho) has a small impact on infrared emissivity due to their similar characteristics to La³⁺ and Pr³⁺. Our findings provide a valuable reference for achieving high-performance infrared emission in rare-earth cerates through doping engineering.</div></div>","PeriodicalId":18253,"journal":{"name":"Materials Today Physics","volume":"50 ","pages":"Article 101615"},"PeriodicalIF":10.0,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142782495","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}

{"title":"Computational investigation of NaKFePO4F fluorophosphate as a high-performance cathode material for Na/K-ion batteries","authors":"Abdelghani Bensassi ,&nbsp;Zineb El Kacemi ,&nbsp;Zouhir Mansouri ,&nbsp;Abdelfattah Mahmoud ,&nbsp;Mohamed Balli ,&nbsp;Abdallah El Kenz ,&nbsp;Abdelilah Benyoussef ,&nbsp;Omar Mounkachi","doi":"10.1016/j.mtphys.2024.101623","DOIUrl":"10.1016/j.mtphys.2024.101623","url":null,"abstract":"<div><div>Recently, NaKFePO₄F, a layered iron-based fluorophosphate, has been proposed as a promising cathode material for both sodium-ion (SIBs) and potassium-ion batteries (KIBs), with an ion-exchange strategy significantly enhancing its capacity and addressing its low electronic conductivity. However, the atomic-scale mechanisms driving these improvements have yet to be fully explained. For this reason, density functional theory (DFT) and ab initio molecular dynamics (AIMD) simulations were systematically employed to assess the electrochemical feasibility of NaKFePO₄F as a novel cathode material for these batteries. Analysis of energetically stable configurations reveals that a 50 % exchange of Na with K stabilizes and activates the previously inert sites in the pristine Na₂FePO₄F material. Notably, NaKFePO₄F exhibits enhanced thermodynamic stability and electronic conductivity, with a reduced band gap of 2.40 eV compared to 3.18 eV in the pristine material. Moreover, NaKFePO₄F was found to exhibit a low activation energy barrier of 0.42 eV for K ions, as determined by climbing image nudged elastic band (CI-NEB) computations. AIMD predictions also indicate that this material can sustain elevated temperatures from 300 K to 800 K, with ion diffusivity described accordingly. Ultimately, NaKFePO₄F achieved an average discharge voltage of 3.67 V and an energy density of 426 Wh/kg for KIBs, surpassing the 3.49 V discharge voltage and 405 Wh/kg energy density of SIBs. Given these predicted results, NaKFePO₄F is expected to be a promising cathode material for post-lithium-ion battery technology.</div></div>","PeriodicalId":18253,"journal":{"name":"Materials Today Physics","volume":"50 ","pages":"Article 101623"},"PeriodicalIF":10.0,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142804676","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}

{"title":"Rapid prediction of phonon density of states by crystal attention graph neural network and high-throughput screening of candidate substrates for wide bandgap electronic cooling","authors":"Mohammed Al-Fahdi ,&nbsp;Changpeng Lin ,&nbsp;Chen Shen ,&nbsp;Hongbin Zhang ,&nbsp;Ming Hu","doi":"10.1016/j.mtphys.2024.101632","DOIUrl":"10.1016/j.mtphys.2024.101632","url":null,"abstract":"<div><div>Machine learning has demonstrated superior performance in predicting vast materials properties. However, predicting a spectral-like continuous material property such as phonon density of states (DOS) is more challenging for machine learning. In this work, with phonon DOS of 4994 inorganic structures with 62 unique elements calculated by density functional theory (DFT), we developed a crystal attention graph neural network (CATGNN) model for predicting total phonon DOS of crystalline materials. The computational cost of training the CATGNN model is several orders of magnitude cheaper than full DFT calculations. We find that high vibrational similarity or phonon DOS overlap is not the only requirement to obtain high interfacial thermal conductance (ITC) instead, the average acoustic group velocity of heat source and heat sink for the acoustic branches in the phonon DOS overlap region is equally important in determining ITC. Pearson correlation analysis yields a few simple material descriptors that are strongly but negatively correlated with ITC. These easy-to-calculate material features combined with the proposed high average acoustic group velocity and phonon DOS overlap predicted by CATGNN model offer a new reliable and fast route for high-throughput screening of novel crystalline materials with desirable high ITC for phonon-mediated thermal management of wide bandgap electronics.</div></div>","PeriodicalId":18253,"journal":{"name":"Materials Today Physics","volume":"50 ","pages":"Article 101632"},"PeriodicalIF":10.0,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142857909","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}

{"title":"Insights into the enhanced ORR activity of FeN4-embedded graphene through interface interactions with metal substrates: Electronic vs. geometric descriptors","authors":"Silu Li ,&nbsp;Donghai Wu ,&nbsp;Lulu Gao ,&nbsp;Jiahang Li ,&nbsp;Gang Tang ,&nbsp;Zaiping Zeng ,&nbsp;Dongwei Ma","doi":"10.1016/j.mtphys.2024.101633","DOIUrl":"10.1016/j.mtphys.2024.101633","url":null,"abstract":"<div><div>Recent experiments have revealed that the oxygen reduction reaction (ORR) performances of transition-metal and nitrogen codoped carbon (TM-N-C) can be drastically improved by interfacing with TM nanoparticles. However, the key factors that derive from this emerging composite SAC and can well correlate with the boosted ORR activity is still unclear. Herein, taking the FeN₄-embedded graphene (FeN₄-G) as example, we built a series of model heterointerface systems, by placing FeN₄-G on various common TM surfaces (denoted as FeN₄-M), to explore the enhancement origin. Based on extensive density functional theory calculations, we find that all the FeN₄-M systems exhibit higher ORR activity than the free-standing FeN₄-G, and even most FeN₄-M systems are much more active than the Pt(111) surface. Furthermore, for the descriptor construction, however there is no apparent correlation between the ORR activity and the electronic structures of Fe active centers, the ones that are closely relevant with ORR activity of the free-standing FeN₄-G. Instead, interestingly the interlayer distance between FeN₄-G and the underlying metal substrates, an intrinsic geometric structure parameter, has been identified to linearly correlate with the binding strengths of ORR intermediates and ORR overpotential well. Present work provides a novel insight into the structure-activity relationship of the composite SACs consisting of Fe-N-C and metal nanoparticles.</div></div>","PeriodicalId":18253,"journal":{"name":"Materials Today Physics","volume":"50 ","pages":"Article 101633"},"PeriodicalIF":10.0,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142857910","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}