Pub Date : 2025-04-30DOI: 10.1016/j.apmate.2025.100298
Jinfeng Xu , Yu Meng , Xiaoyi Qiu , Hong Zhong , Shaokang Liu , Lili Zhang , Jiayang Zhang , Pengxiang Hou , Scott P. Beckman , Feng Wu , Chang Liu , Minhua Shao , Jincheng Li
The great interest of Fe-N/C based Zn-air batteries and fuel cells intrigues large numbers of studies on modulating the pore structure for fast mass transport and the electronic structure of atomic Fe centers for enhancing intrinsic activity for oxygen reduction reaction (ORR). A Zn-assisted strategy herein is developed to synthesize a honeycomb-like micro-nanoscale porous Fe-N/C catalyst with atomic FeN3Cl active sites. Specifically, Zn-guided synthesis of honeycomb-like porous carbon supported ZnO, ZnO-templated assembly of hemin modified ZIF-8 on honeycomb-like carbon and Zn/ZnO-assisted pyrolysis of the ZIF-8 precursor are involved. The synthetic mechanism is revealed by in-situ transmission electron microscopy imaging and in-situ X-ray diffraction analysis. Density functional theory calculations demonstrate FeN3Cl can prominently lower the ORR energy barrier on the Fe centers, greatly facilitating catalytic kinetics. Hence, high ORR performance, including half-wave potentials of 0.81 V in acidic conditions and 0.91 V under alkaline media, is achieved. Besides, Zn-air batteries and H2-O2 fuel cells base on the resulting catalyst are investigated, also exhibiting excellent battery/cell performances. This study provides a novel strategy for the preparation of honeycomb-like micro-nanoscale porous single-atom catalysts as well as a significant new insight on the catalytic mechanisms, helping to advance in energy devices.
基于Fe- n /C的锌空气电池和燃料电池引起了人们的极大兴趣，人们对其进行了大量的研究，以调节快速质量传递的孔结构和原子铁中心的电子结构，以提高氧还原反应（ORR）的固有活性。本文提出了一种锌辅助策略来合成具有原子FeN3Cl活性位点的蜂窝状微纳米级多孔Fe-N/C催化剂。具体而言，研究包括：Zn引导下蜂窝状多孔碳负载ZnO的合成、ZnO模板化修饰ZIF-8在蜂窝状碳上的组装以及Zn/ZnO辅助ZIF-8前驱体的热解。通过原位透射电镜成像和原位x射线衍射分析揭示了合成机理。密度泛函理论计算表明，FeN3Cl显著降低了Fe中心的ORR能垒，极大地促进了催化动力学。因此，实现了高ORR性能，包括在酸性条件下的0.81 V和在碱性介质下的0.91 V的半波电位。此外，还研究了基于该催化剂的锌空气电池和H2-O2燃料电池，均表现出优异的电池/电池性能。该研究为蜂窝状微纳米多孔单原子催化剂的制备提供了新的策略，并对催化机理有了重要的新认识，有助于推进能源器件的发展。
{"title":"Honeycomb-like single-atom catalysts with FeN3Cl sites for high-performance oxygen reduction","authors":"Jinfeng Xu , Yu Meng , Xiaoyi Qiu , Hong Zhong , Shaokang Liu , Lili Zhang , Jiayang Zhang , Pengxiang Hou , Scott P. Beckman , Feng Wu , Chang Liu , Minhua Shao , Jincheng Li","doi":"10.1016/j.apmate.2025.100298","DOIUrl":"10.1016/j.apmate.2025.100298","url":null,"abstract":"<div><div>The great interest of Fe-N/C based Zn-air batteries and fuel cells intrigues large numbers of studies on modulating the pore structure for fast mass transport and the electronic structure of atomic Fe centers for enhancing intrinsic activity for oxygen reduction reaction (ORR). A Zn-assisted strategy herein is developed to synthesize a honeycomb-like micro-nanoscale porous Fe-N/C catalyst with atomic FeN<sub>3</sub>Cl active sites. Specifically, Zn-guided synthesis of honeycomb-like porous carbon supported ZnO, ZnO-templated assembly of hemin modified ZIF-8 on honeycomb-like carbon and Zn/ZnO-assisted pyrolysis of the ZIF-8 precursor are involved. The synthetic mechanism is revealed by <em>in-situ</em> transmission electron microscopy imaging and <em>in-situ</em> X-ray diffraction analysis. Density functional theory calculations demonstrate FeN<sub>3</sub>Cl can prominently lower the ORR energy barrier on the Fe centers, greatly facilitating catalytic kinetics. Hence, high ORR performance, including half-wave potentials of 0.81 V in acidic conditions and 0.91 V under alkaline media, is achieved. Besides, Zn-air batteries and H<sub>2</sub>-O<sub>2</sub> fuel cells base on the resulting catalyst are investigated, also exhibiting excellent battery/cell performances. This study provides a novel strategy for the preparation of honeycomb-like micro-nanoscale porous single-atom catalysts as well as a significant new insight on the catalytic mechanisms, helping to advance in energy devices.</div></div>","PeriodicalId":7283,"journal":{"name":"Advanced Powder Materials","volume":"4 4","pages":"Article 100298"},"PeriodicalIF":0.0,"publicationDate":"2025-04-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144155021","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-04-17DOI: 10.1016/j.apmate.2025.100297
Xiaodong Lv , Ting Han , Rong Liu , Fengyu Li , Jian Gong , Zhongfang Chen
Pursuing new two-dimensional (2D) materials has been a hot topic in materials science, driven by their potential for diverse applications. Recent research has unveiled stable planar hypercoordinate motifs with unconventional geometric arrangements and bonding patterns that facilitate the synthesis of new 2D materials with diverse applications. Among these, yet the design of 2D transition metal systems featuring planar pentacoordinate boron (ppB) is particularly intriguing. Here we address this gap by proposing a novel family of transition metal boride monolayers (MBenes) composed of ppB and heptacoordinate M motifs. The novelty of our MBenes stems from their distinct atomic arrangements and bonding configurations, setting them apart from traditional 2D materials. High-throughput calculations identified 10 stable MBenes (with the stoichiometry of MB, M = Cr, Fe, Co, Ni, Cu, Mo, Pd, Ag, Pt, Au) with exceptional thermodynamic, dynamic, thermal, and mechanical stabilities attributed to strong B−B covalent bonds and M−B ionic interactions. Notably, five of these MBenes (M = Ni, Pd, Pt, Ag, Au) hold high promise as topological superconducting materials with superconducting transition temperatures of 2.4–5.2 K. This discovery not only enriches the family of topological superconducting materials but also opens new avenues for quantum device development. Meanwhile, FeB monolayer exhibits robust ferromagnetic properties with a high Curie temperature of ∼750 K, which is particularly significant for spintronics applications. In addition, NiB and CuB MBenes demonstrate extremely low sodium diffusion barriers (about 30 and 90 meV) and high sodium storage capacities (788 and 734 mAh g−1, respectively), making them promising anode materials for sodium-ion batteries (SIBs). This study expands the selection of electrode materials for SIBs and mitigates some existing limitations in battery technology. Overall, these findings underscore the multifunctional potential of MBenes, positioning them as transformative materials for quantum computing, spintronics, and energy storage applications.
{"title":"High-throughput theoretical exploration of multifunctional planar MBenes: Magnetism, topology, superconductivity, and anode applications","authors":"Xiaodong Lv , Ting Han , Rong Liu , Fengyu Li , Jian Gong , Zhongfang Chen","doi":"10.1016/j.apmate.2025.100297","DOIUrl":"10.1016/j.apmate.2025.100297","url":null,"abstract":"<div><div>Pursuing new two-dimensional (2D) materials has been a hot topic in materials science, driven by their potential for diverse applications. Recent research has unveiled stable planar hypercoordinate motifs with unconventional geometric arrangements and bonding patterns that facilitate the synthesis of new 2D materials with diverse applications. Among these, yet the design of 2D transition metal systems featuring planar pentacoordinate boron (ppB) is particularly intriguing. Here we address this gap by proposing a novel family of transition metal boride monolayers (MBenes) composed of ppB and heptacoordinate M motifs. The novelty of our MBenes stems from their distinct atomic arrangements and bonding configurations, setting them apart from traditional 2D materials. High-throughput calculations identified 10 stable MBenes (with the stoichiometry of MB, M = Cr, Fe, Co, Ni, Cu, Mo, Pd, Ag, Pt, Au) with exceptional thermodynamic, dynamic, thermal, and mechanical stabilities attributed to strong B−B covalent bonds and M−B ionic interactions. Notably, five of these MBenes (M = Ni, Pd, Pt, Ag, Au) hold high promise as topological superconducting materials with superconducting transition temperatures of 2.4–5.2 K. This discovery not only enriches the family of topological superconducting materials but also opens new avenues for quantum device development. Meanwhile, FeB monolayer exhibits robust ferromagnetic properties with a high Curie temperature of ∼750 K, which is particularly significant for spintronics applications. In addition, NiB and CuB MBenes demonstrate extremely low sodium diffusion barriers (about 30 and 90 meV) and high sodium storage capacities (788 and 734 mAh g<sup>−1</sup>, respectively), making them promising anode materials for sodium-ion batteries (SIBs). This study expands the selection of electrode materials for SIBs and mitigates some existing limitations in battery technology. Overall, these findings underscore the multifunctional potential of MBenes, positioning them as transformative materials for quantum computing, spintronics, and energy storage applications.</div></div>","PeriodicalId":7283,"journal":{"name":"Advanced Powder Materials","volume":"4 3","pages":"Article 100297"},"PeriodicalIF":0.0,"publicationDate":"2025-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143885946","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","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.apmate.2025.100296
Renfei Zhao , Yuanhang Gao , Zuosu Qin , Yuelin Li , Tao Zhang , Anqiang Pan , Ning Zhang , Renzhi Ma , Xiaohe Liu , Gen Chen
The poor oxidation stability of ether-based solvents has long been a major challenge limiting their practical application. To enhance the oxidative stability of ether-based electrolytes, the physicochemical properties of various glycol dimethyl ethers are screened, and diglyme (G2) is selected as the sole solvent for the electrolyte. Lithium bis(fluorosulfonyl)imide (LiFSI), a highly dissociative salt, is used as the primary salt; while lithium nitrate (LiNO3) and lithium difluorophosphate (LiDFP), which have small ionic sizes and strong binding energies, are added as secondary salts. The resulting electrolyte can modulate the electric double layer structure by NO3− and DFP− on the cathode side, leading to an increased Li+ concentration that is originally repelled by the cathode. Additionally, the oxidation stability of the electrolyte is improved and the formed electrode-electrolyte interphase is more uniform and stable, thereby enhancing the electrochemical performance of the cells. As a result, cells assembled with a total of 1 M ternary lithium salts in G2 solvent can operate at high voltage of 4.4 V. The Li||NCM811 cells maintain 80.2% capacity retention after 270 cycles at room temperature, with an average Coulombic efficiency of 99.5%, and exhibit 88.4% capacity retention after 200 cycles at −30 °C.
{"title":"Regulating electric double layer in non-fluorinated ether electrolyte enables high-voltage and low-temperature lithium metal batteries","authors":"Renfei Zhao , Yuanhang Gao , Zuosu Qin , Yuelin Li , Tao Zhang , Anqiang Pan , Ning Zhang , Renzhi Ma , Xiaohe Liu , Gen Chen","doi":"10.1016/j.apmate.2025.100296","DOIUrl":"10.1016/j.apmate.2025.100296","url":null,"abstract":"<div><div>The poor oxidation stability of ether-based solvents has long been a major challenge limiting their practical application. To enhance the oxidative stability of ether-based electrolytes, the physicochemical properties of various glycol dimethyl ethers are screened, and diglyme (G2) is selected as the sole solvent for the electrolyte. Lithium bis(fluorosulfonyl)imide (LiFSI), a highly dissociative salt, is used as the primary salt; while lithium nitrate (LiNO<sub>3</sub>) and lithium difluorophosphate (LiDFP), which have small ionic sizes and strong binding energies, are added as secondary salts. The resulting electrolyte can modulate the electric double layer structure by NO<sub>3</sub><sup>−</sup> and DFP<sup>−</sup> on the cathode side, leading to an increased Li<sup>+</sup> concentration that is originally repelled by the cathode. Additionally, the oxidation stability of the electrolyte is improved and the formed electrode-electrolyte interphase is more uniform and stable, thereby enhancing the electrochemical performance of the cells. As a result, cells assembled with a total of 1 M ternary lithium salts in G2 solvent can operate at high voltage of 4.4 V. The Li||NCM811 cells maintain 80.2% capacity retention after 270 cycles at room temperature, with an average Coulombic efficiency of 99.5%, and exhibit 88.4% capacity retention after 200 cycles at −30 °C.</div></div>","PeriodicalId":7283,"journal":{"name":"Advanced Powder Materials","volume":"4 3","pages":"Article 100296"},"PeriodicalIF":0.0,"publicationDate":"2025-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143899386","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-04-15DOI: 10.1016/j.apmate.2025.100295
Ye Chen , Shilong Li , Congxin Xia , Miao Tian , Yaxin Guo , Xupo Liu , Mingjin Cui , Shixue Dou , Hanleem Lee , Vadivel Subramaniam , Krishnamoorthy Ramachandran , Xinghui Liu
Carbon-based low-dimensional materials (CLDM) with elemental carbon as the main component have unique physical and chemical properties, and become the focus of research in many fields including energy, environmental protection, and information technology. Notably, cellulose acetate, the main component of cigarette butts (CBs), is a one-dimensional precursor with a large specific surface area and aspect ratio. Still, their usefulness as building fillers has often been underestimated before. This review summarizes recent advances in CBs recycling and provides suggested guidelines for its use as a CLDM material in renewable energy. Specifically, we first describe the harmful effects of CBs as pollutants in our lives to emphasize the importance of proper recycling. We then summarize previous methods of recycling CBs waste, including clay bricks, asphalt concrete pavement, gypsum, acoustic materials, chemisorption, vector control, and corrosion control. The potential applications of CBs include triboelectric nanogenerator applications, flexible batteries, enhanced metal-organic framework material energy storage devices, and carbon-based hydrogen storage. Finally, the advantages of utilizing CBs-derived CLDM materials over conventional solutions in the energy field are discussed. This review will provide new avenues for solving the intractable problem of CBs and reducing the manufacturing costs of renewable materials.
{"title":"Exploring the potential of low-dimensional materials from cigarette butts for energy applications: A comprehensive review","authors":"Ye Chen , Shilong Li , Congxin Xia , Miao Tian , Yaxin Guo , Xupo Liu , Mingjin Cui , Shixue Dou , Hanleem Lee , Vadivel Subramaniam , Krishnamoorthy Ramachandran , Xinghui Liu","doi":"10.1016/j.apmate.2025.100295","DOIUrl":"10.1016/j.apmate.2025.100295","url":null,"abstract":"<div><div>Carbon-based low-dimensional materials (CLDM) with elemental carbon as the main component have unique physical and chemical properties, and become the focus of research in many fields including energy, environmental protection, and information technology. Notably, cellulose acetate, the main component of cigarette butts (CBs), is a one-dimensional precursor with a large specific surface area and aspect ratio. Still, their usefulness as building fillers has often been underestimated before. This review summarizes recent advances in CBs recycling and provides suggested guidelines for its use as a CLDM material in renewable energy. Specifically, we first describe the harmful effects of CBs as pollutants in our lives to emphasize the importance of proper recycling. We then summarize previous methods of recycling CBs waste, including clay bricks, asphalt concrete pavement, gypsum, acoustic materials, chemisorption, vector control, and corrosion control. The potential applications of CBs include triboelectric nanogenerator applications, flexible batteries, enhanced metal-organic framework material energy storage devices, and carbon-based hydrogen storage. Finally, the advantages of utilizing CBs-derived CLDM materials over conventional solutions in the energy field are discussed. This review will provide new avenues for solving the intractable problem of CBs and reducing the manufacturing costs of renewable materials.</div></div>","PeriodicalId":7283,"journal":{"name":"Advanced Powder Materials","volume":"4 3","pages":"Article 100295"},"PeriodicalIF":0.0,"publicationDate":"2025-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143894883","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-03-27DOI: 10.1016/j.apmate.2025.100288
Xu Zhang , Peng Yu , Di Shen , Bin Cai , Tianyu Han , Ying Xie , Lei Wang
The susceptibility of Pt catalyst surfaces to carbon monoxide (CO) poisoning in anodic hydrogen oxidation reaction (HOR) has been a critical constraint on the development of proton exchange membrane fuel cells (PEMFCs). Effectively regulating the electronic structure of Pt to enhance CO resistance is crucial for developing high-performance catalysts with robust anti-poisoning capabilities. Herein, the Pt/W@NCNF featured by Pt nanoparticles and atomical dispersed tungsten (W) sites on N-doped carbon nanofibers is developed for CO tolerance HOR catalyst. The presence of W enables the electron transfer from Pt, which promotes electron rearrangement in the Pt-5d orbitals. It not only optimizes the adsorption of H∗ and CO∗ on Pt, but also the OH∗ intermediates adsorbed on the W sites oxidize the CO∗ adsorbed on Pt, thereby retaining more active sites for H2 adsorption and oxidation. The HOR exchange current density of Pt/W@NCNF reaches 1.35 times that of commercial Pt/C, and the limiting current density decreases by only 3.4% after introducing 1000 ppm CO in H2. Notably, the Pt/W@NCNF-based PEMFCs deliver markedly superior performance across a range of CO concentrations. The present study demonstrates that electronic modulation of Pt is an effective strategy for simultaneously achieving resistance to CO and promoted HOR activity.
{"title":"Atomically dispersed tungsten enhances CO tolerance in electrocatalytic hydrogen oxidation by regulating the 5d-orbital electrons of platinum","authors":"Xu Zhang , Peng Yu , Di Shen , Bin Cai , Tianyu Han , Ying Xie , Lei Wang","doi":"10.1016/j.apmate.2025.100288","DOIUrl":"10.1016/j.apmate.2025.100288","url":null,"abstract":"<div><div>The susceptibility of Pt catalyst surfaces to carbon monoxide (CO) poisoning in anodic hydrogen oxidation reaction (HOR) has been a critical constraint on the development of proton exchange membrane fuel cells (PEMFCs). Effectively regulating the electronic structure of Pt to enhance CO resistance is crucial for developing high-performance catalysts with robust anti-poisoning capabilities. Herein, the Pt/W@NCNF featured by Pt nanoparticles and atomical dispersed tungsten (W) sites on N-doped carbon nanofibers is developed for CO tolerance HOR catalyst. The presence of W enables the electron transfer from Pt, which promotes electron rearrangement in the Pt-5d orbitals. It not only optimizes the adsorption of H∗ and CO∗ on Pt, but also the OH∗ intermediates adsorbed on the W sites oxidize the CO∗ adsorbed on Pt, thereby retaining more active sites for H<sub>2</sub> adsorption and oxidation. The HOR exchange current density of Pt/W@NCNF reaches 1.35 times that of commercial Pt/C, and the limiting current density decreases by only 3.4% after introducing 1000 ppm CO in H<sub>2</sub>. Notably, the Pt/W@NCNF-based PEMFCs deliver markedly superior performance across a range of CO concentrations. The present study demonstrates that electronic modulation of Pt is an effective strategy for simultaneously achieving resistance to CO and promoted HOR activity.</div></div>","PeriodicalId":7283,"journal":{"name":"Advanced Powder Materials","volume":"4 3","pages":"Article 100288"},"PeriodicalIF":0.0,"publicationDate":"2025-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143814832","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-03-26DOI: 10.1016/j.apmate.2025.100286
Xiaona Li , Hang Luo , Di Zhai , Yuting Wan , Guanghu He , Deng Hu , Hongshuai Hou , Dou Zhang , Shujun Zhang
Polymer dielectrics possessing excellent electrical insulation and high thermal conductivity are pivotal for dielectric capacitors at elevated temperatures. However, the integration of electrical insulation and thermal conductivity in polymers remains a challenge. In this work, we present a feasible strategy to integrate high electrical insulation and high thermal conductivity by bonding carbon quantum dots (CQDs) with the diamine monomer of polyetherimide (PEI). The CQDs with Coulomb blockade effect serve as traps for the migrating of electrons in the dielectrics, while the bonding networks formed by CQDs and PEI further deepen the traps and augment trap density. As a result, the hybrid dielectrics (PEI-NH2-CQDs) exhibit nearly an order of magnitude higher electrical resistivity than that of pure PEI, leading to an 80% increase in discharge energy density with an energy efficiency of 90% at 200 °C compared to pure counterpart. Additionally, this all-organic dielectric achieves a significantly increased thermal conductivity of 0.65 W m−1 K−1 compared to 0.26 W m−1 K−1 of PEI, which supports its cyclic stability at elevated temperatures. We also demonstrate the kilogram-scale production of CQDs, synthesizing over 8 kg in a single batch, paving the way for large-scale production of reliable PEI-NH2-CQDs dielectrics.
聚合物电介质具有出色的电气绝缘性和高导热性，对于高温下的电介质电容器至关重要。然而，如何在聚合物中集成电绝缘和热导率仍然是一项挑战。在这项工作中，我们提出了一种可行的策略，通过将碳量子点（CQDs）与聚醚酰亚胺（PEI）的二胺单体结合，实现高电绝缘和高导热性的整合。具有库仑封锁效应的碳量子点是电介质中电子迁移的陷阱，而碳量子点与 PEI 形成的键合网络则进一步加深了陷阱并提高了陷阱密度。因此，混合电介质（PEI-NH2-CQDs）的电阻率比纯 PEI 高出近一个数量级，与纯 PEI 相比，放电能量密度提高了 80%，200 °C 时的能量效率达到 90%。此外，与 PEI 的 0.26 W m-1 K-1 相比，这种全有机电介质的热导率显著提高，达到 0.65 W m-1 K-1，这支持了它在高温下的循环稳定性。我们还展示了公斤级的 CQDs 生产，单批合成量超过 8 公斤，为大规模生产可靠的 PEI-NH2-CQDs 电介质铺平了道路。
{"title":"Enhanced capacitive energy storage of polyetherimide at high temperatures by integration of electrical insulation and thermal conductivity","authors":"Xiaona Li , Hang Luo , Di Zhai , Yuting Wan , Guanghu He , Deng Hu , Hongshuai Hou , Dou Zhang , Shujun Zhang","doi":"10.1016/j.apmate.2025.100286","DOIUrl":"10.1016/j.apmate.2025.100286","url":null,"abstract":"<div><div>Polymer dielectrics possessing excellent electrical insulation and high thermal conductivity are pivotal for dielectric capacitors at elevated temperatures. However, the integration of electrical insulation and thermal conductivity in polymers remains a challenge. In this work, we present a feasible strategy to integrate high electrical insulation and high thermal conductivity by bonding carbon quantum dots (CQDs) with the diamine monomer of polyetherimide (PEI). The CQDs with Coulomb blockade effect serve as traps for the migrating of electrons in the dielectrics, while the bonding networks formed by CQDs and PEI further deepen the traps and augment trap density. As a result, the hybrid dielectrics (PEI-NH<sub>2</sub>-CQDs) exhibit nearly an order of magnitude higher electrical resistivity than that of pure PEI, leading to an 80% increase in discharge energy density with an energy efficiency of 90% at 200 °C compared to pure counterpart. Additionally, this all-organic dielectric achieves a significantly increased thermal conductivity of 0.65 W m<sup>−1</sup> K<sup>−1</sup> compared to 0.26 W m<sup>−1</sup> K<sup>−1</sup> of PEI, which supports its cyclic stability at elevated temperatures. We also demonstrate the kilogram-scale production of CQDs, synthesizing over 8 kg in a single batch, paving the way for large-scale production of reliable PEI-NH<sub>2</sub>-CQDs dielectrics.</div></div>","PeriodicalId":7283,"journal":{"name":"Advanced Powder Materials","volume":"4 3","pages":"Article 100286"},"PeriodicalIF":0.0,"publicationDate":"2025-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143783900","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-03-26DOI: 10.1016/j.apmate.2025.100287
Wenjian Guo , Fayuan Li , Lingyu Wang , Li'an Zhu , Yicong Ye , Zhen Wang , Bin Yang , Shifeng Zhang , Shuxin Bai
In materials science, a significant correlation often exists between material input parameters and their corresponding performance attributes. Nevertheless, the inherent challenges associated with small data obscure these statistical correlations, impeding machine learning models from effectively capturing the underlying patterns, thereby hampering efficient optimization of material properties. This work presents a novel active learning framework that integrates generative adversarial networks (GAN) with a directionally constrained expected absolute improvement (EAI) acquisition function to accelerate the discovery of ultra-high temperature ceramics (UHTCs) using small data. The framework employs GAN for data augmentation, symbolic regression for feature weight derivation, and a self-developed EAI function that incorporates input feature importance weighting to quantify bidirectional deviations from zero ablation rate. Through only two iterations, this framework successfully identified the optimal composition of HfB2-3.52SiC-5.23TaSi2, which exhibits robust near-zero ablation rates under plasma ablation at 2500 °C for 200 s, demonstrating superior sampling efficiency compared to conventional active learning approaches. Microstructural analysis reveals that the exceptional performance stems from the formation of a highly viscous HfO2-SiO2-Ta2O5-HfSiO4-Hf3(BO3)4 oxide layer, which provides effective oxygen barrier protection. This work demonstrates an efficient and universal approach for rapid materials discovery using small data.
{"title":"Accelerated discovery of near-zero ablation ultra-high temperature ceramics via GAN-enhanced directionally constrained active learning","authors":"Wenjian Guo , Fayuan Li , Lingyu Wang , Li'an Zhu , Yicong Ye , Zhen Wang , Bin Yang , Shifeng Zhang , Shuxin Bai","doi":"10.1016/j.apmate.2025.100287","DOIUrl":"10.1016/j.apmate.2025.100287","url":null,"abstract":"<div><div>In materials science, a significant correlation often exists between material input parameters and their corresponding performance attributes. Nevertheless, the inherent challenges associated with small data obscure these statistical correlations, impeding machine learning models from effectively capturing the underlying patterns, thereby hampering efficient optimization of material properties. This work presents a novel active learning framework that integrates generative adversarial networks (GAN) with a directionally constrained expected absolute improvement (EAI) acquisition function to accelerate the discovery of ultra-high temperature ceramics (UHTCs) using small data. The framework employs GAN for data augmentation, symbolic regression for feature weight derivation, and a self-developed EAI function that incorporates input feature importance weighting to quantify bidirectional deviations from zero ablation rate. Through only two iterations, this framework successfully identified the optimal composition of HfB<sub>2</sub>-3.52SiC-5.23TaSi<sub>2</sub>, which exhibits robust near-zero ablation rates under plasma ablation at 2500 °C for 200 s, demonstrating superior sampling efficiency compared to conventional active learning approaches. Microstructural analysis reveals that the exceptional performance stems from the formation of a highly viscous HfO<sub>2</sub>-SiO<sub>2</sub>-Ta<sub>2</sub>O<sub>5</sub>-HfSiO<sub>4</sub>-Hf<sub>3</sub>(BO<sub>3</sub>)<sub>4</sub> oxide layer, which provides effective oxygen barrier protection. This work demonstrates an efficient and universal approach for rapid materials discovery using small data.</div></div>","PeriodicalId":7283,"journal":{"name":"Advanced Powder Materials","volume":"4 3","pages":"Article 100287"},"PeriodicalIF":0.0,"publicationDate":"2025-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143814831","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-03-21DOI: 10.1016/j.apmate.2025.100284
Khakemin Khan , Ahmed Mahmood Idris , Haseebul Hassan , Sajjad Haider , Salah Ud-Din Khan , Antonio Miotello , Ihsanullah Khan
Simultaneously inducing dual built-in electric fields (EFs) both within a single component and at the heterojunction interface creates a dual-driving force that is crucial for promoting spatial charge separation. This is particularly significant in challenging coupled systems, such as CO2 photoreduction integrated with selective oxidation of toluene to benzaldehyde. However, developing such a system is quite challenging and often requires a precise design and engineering. Herein, we demonstrate a unique Ni-CdS@Ni(OH)2 heterojunction synthesized via an in-situ self-assembly method. Comprehensive mechanistic and theoretical investigations reveal that the Ni-CdS@Ni(OH)2 heterojunction induces dual electric fields (EFs): an intrinsic polarized electric-field within the CdS lattice from Ni doping and an interfacial electric-field from the growth of ultrathin nanosheets of Ni(OH)2 on Ni-CdS nanorods, enabling efficient spatial charge separation and enhanced redox potential. As proof of concept, the Ni-CdS@Ni(OH)2 heterojunction simultaneously exhibits outstanding bifunctional photocatalytic performance, producing CO at a rate of 427 μmol g−1 h−1 and selectively oxidizing toluene to benzaldehyde at a rate of 1476 μmol g−1 h−1 with a selectivity exceeding 85%. This work offers a promising strategy to optimize the utilization of photogenerated carriers in heterojunction photocatalysts, advancing synergistic photocatalytic redox systems.
{"title":"Dual electric fields in Ni-CdS@Ni(OH)2 heterojunction: A synergistic spatial charge separation approach for enhanced coupled CO2 photoreduction and selective toluene oxidation","authors":"Khakemin Khan , Ahmed Mahmood Idris , Haseebul Hassan , Sajjad Haider , Salah Ud-Din Khan , Antonio Miotello , Ihsanullah Khan","doi":"10.1016/j.apmate.2025.100284","DOIUrl":"10.1016/j.apmate.2025.100284","url":null,"abstract":"<div><div>Simultaneously inducing dual built-in electric fields (EFs) both within a single component and at the heterojunction interface creates a dual-driving force that is crucial for promoting spatial charge separation. This is particularly significant in challenging coupled systems, such as CO<sub>2</sub> photoreduction integrated with selective oxidation of toluene to benzaldehyde. However, developing such a system is quite challenging and often requires a precise design and engineering. Herein, we demonstrate a unique Ni-CdS@Ni(OH)<sub>2</sub> heterojunction synthesized via an <em>in-situ</em> self-assembly method. Comprehensive mechanistic and theoretical investigations reveal that the Ni-CdS@Ni(OH)<sub>2</sub> heterojunction induces dual electric fields (EFs): an intrinsic polarized electric-field within the CdS lattice from Ni doping and an interfacial electric-field from the growth of ultrathin nanosheets of Ni(OH)<sub>2</sub> on Ni-CdS nanorods, enabling efficient spatial charge separation and enhanced redox potential. As proof of concept, the Ni-CdS@Ni(OH)<sub>2</sub> heterojunction simultaneously exhibits outstanding bifunctional photocatalytic performance, producing CO at a rate of 427 μmol g<sup>−1</sup> h<sup>−1</sup> and selectively oxidizing toluene to benzaldehyde at a rate of 1476 μmol g<sup>−1</sup> h<sup>−1</sup> with a selectivity exceeding 85%. This work offers a promising strategy to optimize the utilization of photogenerated carriers in heterojunction photocatalysts, advancing synergistic photocatalytic redox systems.</div></div>","PeriodicalId":7283,"journal":{"name":"Advanced Powder Materials","volume":"4 3","pages":"Article 100284"},"PeriodicalIF":0.0,"publicationDate":"2025-03-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143799737","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-03-18DOI: 10.1016/j.apmate.2025.100283
Yiming Xia , Nilotpal Kapuria , Mingrui He , Uma V. Ghorpade , Xinyao Guo , Bohan Hao , Seung Wook Shin , Ziv Hameiri , Xiaojing Hao , Mahesh P. Suryawanshi
The discovery of quantum dots (QDs) stands as one of the paramount technological breakthroughs of the 20th century. Their versatility spans from everyday applications to cutting-edge scientific research, encompassing areas such as displays, lighting, photocatalysis, bio-imaging, and photonics devices and so on. Among the myriad QDs technologies, industrially relevant CuInS2 (CIS) QDs have emerged as promising alternatives to traditional Cd- and Pb-based QDs. Their tunable optoelectronic properties, high absorption coefficient, compositional flexibility, remarkable stability as well as Restriction of Hazardous Substances-compliance, with recent trends revealing a renewed interest in this material for various visible and near-infrared technological applications. This review focuses on recent advancements in CIS QDs as multidisciplinary field from its genesis in the mid-1990 to date with an emphasis on key breakthroughs in their synthesis, surface chemistry, post-synthesis modifications, and various applications. First, the comparation of properties of CIS QDs with relevant knowledge from other classes of QDs and from I-III-VI semiconductors as well is summarized. Second, recent advances in the synthesis methods, structure-optoelectronic properties, their defects, and passivation strategies as well as CIS-based heterostructures are discussed. Third, the state-of-the-art applications of CIS QDs ranging from solar cells, luminescence solar concentrations, photocatalysis, light emitting diodes, bioimaging and some emerging applications are summarized. Finally, we discuss open challenges and future perspectives for further advancement in this field.
{"title":"Copper indium sulfide colloidal quantum dots: Advances in synthesis, structure-optoelectronic properties, and applications","authors":"Yiming Xia , Nilotpal Kapuria , Mingrui He , Uma V. Ghorpade , Xinyao Guo , Bohan Hao , Seung Wook Shin , Ziv Hameiri , Xiaojing Hao , Mahesh P. Suryawanshi","doi":"10.1016/j.apmate.2025.100283","DOIUrl":"10.1016/j.apmate.2025.100283","url":null,"abstract":"<div><div>The discovery of quantum dots (QDs) stands as one of the paramount technological breakthroughs of the 20th century. Their versatility spans from everyday applications to cutting-edge scientific research, encompassing areas such as displays, lighting, photocatalysis, bio-imaging, and photonics devices and so on. Among the myriad QDs technologies, industrially relevant CuInS<sub>2</sub> (CIS) QDs have emerged as promising alternatives to traditional Cd- and Pb-based QDs. Their tunable optoelectronic properties, high absorption coefficient, compositional flexibility, remarkable stability as well as Restriction of Hazardous Substances-compliance, with recent trends revealing a renewed interest in this material for various visible and near-infrared technological applications. This review focuses on recent advancements in CIS QDs as multidisciplinary field from its genesis in the mid-1990 to date with an emphasis on key breakthroughs in their synthesis, surface chemistry, post-synthesis modifications, and various applications. First, the comparation of properties of CIS QDs with relevant knowledge from other classes of QDs and from I-III-VI semiconductors as well is summarized. Second, recent advances in the synthesis methods, structure-optoelectronic properties, their defects, and passivation strategies as well as CIS-based heterostructures are discussed. Third, the state-of-the-art applications of CIS QDs ranging from solar cells, luminescence solar concentrations, photocatalysis, light emitting diodes, bioimaging and some emerging applications are summarized. Finally, we discuss open challenges and future perspectives for further advancement in this field.</div></div>","PeriodicalId":7283,"journal":{"name":"Advanced Powder Materials","volume":"4 3","pages":"Article 100283"},"PeriodicalIF":0.0,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143791339","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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