Hybrid journal (It can contain Open Access articles) ISSN (Print) 2095-5138 - ISSN (Online) 2053-714X Published by Oxford University Press[425 journals]
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First page: nwae233 Abstract: ABSTRACTPlatinum-based intermetallic compounds (IMCs) play a vital role as electrocatalysts in a range of energy and environmental technologies, such as proton exchange membrane fuel cells. However, the synthesis of IMCs necessitates recombination of ordered Pt-M metallic bonds with high temperature driving, which is generally accompanied by side effects for catalysts’ structure and performance. In this work, we highlight that semimetal atoms can trigger covalent interactions to break the synthesis-temperature limitation of platinum-based intermetallic compounds and benefit fuel-cell electrocatalysis. Attributed to partial fillings of p-block in semimetal elements, the strong covalent interaction of d-p π backbonding can benefit the recombination of ordered Pt-M metallic bonds (PtGe, PtSb and PtTe) in the synthesis process. Moreover, this covalent interaction in metallic states can further promote both electron transport and orbital fillings of active sites in fuel cells. The semimetal-Pt IMCs were obtained with a temperature 300 K lower than that needed for the synthesis of metal-Pt intermetallic compounds and reached the highest CO-tolerant oxygen reduction activity (0.794 A mg−1 at 0.9 V and 5.1% decay under CO poisoning) among reported electrocatalysts. We anticipate that semimetal-Pt IMCs will offer new insights for the rational design of advanced electrocatalysts for fuel cells. PubDate: Mon, 08 Jul 2024 00:00:00 GMT DOI: 10.1093/nsr/nwae233 Issue No:Vol. 11, No. 8 (2024)
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First page: nwae234 Abstract: ABSTRACTRuthenium polypyridyl complexes are promising anticancer candidates, while their cellular targets have rarely been identified, which limits their clinical application. Herein, we design a series of Ru(II) polypyridyl complexes containing bioactive β-carboline derivatives as ligands for anticancer evaluation, among which Ru5 shows suitable lipophilicity, high aqueous solubility, relatively high anticancer activity and cancer cell selectivity. The subsequent utilization of a photo-clickable probe, Ru5a, serves to validate the significance of ATP synthase as a crucial target for Ru5 through photoaffinity-based protein profiling. Ru5 accumulates in mitochondria, impairs mitochondrial functions and induces mitophagy and ferroptosis. Combined analysis of mitochondrial proteomics and RNA-sequencing shows that Ru5 significantly downregulates the expression of the chloride channel protein, and influences genes related to ferroptosis and epithelial-to-mesenchymal transition. Finally, we prove that Ru5 exhibits higher anticancer efficacy than cisplatin in vivo. We firstly identify the molecular targets of ruthenium polypyridyl complexes using a photo-click proteomic method coupled with a multiomics approach, which provides an innovative strategy to elucidate the anticancer mechanisms of metallo-anticancer candidates. PubDate: Fri, 05 Jul 2024 00:00:00 GMT DOI: 10.1093/nsr/nwae234 Issue No:Vol. 11, No. 8 (2024)
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First page: nwae225 Abstract: ABSTRACTPeriodontitis involves hyperactivated stromal cells that recruit immune cells, exacerbating inflammation. This study presents an ATP-responsive metal–organic framework (Mg/Zn-MOF) designed for periodontitis treatment, utilizing ion interference to modulate immune responses and prevent tissue destruction. Addressing the challenges of synergistic ion effects and targeted delivery faced by traditional immunomodulatory nanomaterials, the Mg/Zn-MOF system is activated by extracellular ATP—a pivotal molecule in periodontitis pathology—ensuring targeted ion release. Magnesium and zinc ions released from the framework synergistically inhibit membrane pore formation by attenuating Gasdermin D (GSDMD) expression and activation. This action curtails pyroptosis, lactate dehydrogenase and IL-1β release, thwarting the onset of inflammatory cascades. Mechanistically, Mg/Zn-MOF intervenes in both the NLRP3/Caspase-1/GSDMD and Caspase-11/GSDMD pathways to mitigate pyroptosis. In vivo assessments confirm its effectiveness in diminishing inflammatory cell infiltration and preserving collagen integrity, thereby safeguarding against periodontal tissue damage and bone loss. This investigation highlights the promise of ion-interference strategies in periodontitis immunotherapy, representing a significant stride in developing targeted therapeutic approaches. PubDate: Wed, 26 Jun 2024 00:00:00 GMT DOI: 10.1093/nsr/nwae225 Issue No:Vol. 11, No. 8 (2024)
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First page: nwae218 Abstract: ABSTRACTBoth the catalyst and electrolyte strongly impact the performance of CO2 electrolysis. Despite substantial progress in catalysts, it remains highly challenging to tailor electrolyte compositions and understand their functions at the catalyst interface. Here, we report that the ethylenediaminetetraacetic acid (EDTA) and its analogs, featuring strong Lewis acid-base interaction with metal cations, are selected as electrolyte additives to reshape the catalyst-electrolyte interface for promoting CO2 electrolysis. Mechanistic studies reveal that EDTA molecules are dynamically assembled toward interface regions in response to bias potential due to strong Lewis acid-base interaction of EDTA4–-K+. As a result, the original hydrogen-bond network among interfacial H2O is disrupted, and a hydrogen-bond gap layer at the electrified interface is established. The EDTA-reshaped K+ solvation structure promotes the protonation of *CO2 to *COOH and suppressing *H2O dissociation to *H, thereby boosting the co-electrolysis of CO2 and H2O toward carbon-based products. In particular, when 5 mM of EDTA is added into the electrolytes, the Faradaic efficiency of CO on the commercial Ag nanoparticle catalyst is increased from 57.0% to 90.0% at an industry-relevant current density of 500 mA cm−2. More importantly, the Lewis-base ligand-reshaped interface allows a range of catalysts (Ag, Zn, Pd, Bi, Sn, and Cu) to deliver substantially increased selectivity of carbon-based products in both H-type and flow-type electrolysis cells. PubDate: Sat, 22 Jun 2024 00:00:00 GMT DOI: 10.1093/nsr/nwae218 Issue No:Vol. 11, No. 8 (2024)
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First page: nwae207 Abstract: ABSTRACTThickening of electrodes is crucial for maximizing the proportion of active components and thus improving the energy density of practical energy storage cells. Nevertheless, trade-offs between electrode thickness and electrochemical performance persist because of the considerably increased ion transport resistance of thick electrodes. Herein, we propose accelerating ion transport through thick and dense electrodes by establishing an immobile polyanionic backbone within the electrode pores; and as a proof of concept, gel polyacrylic electrolytes as such a backbone are in situ synthesized for supercapacitors. During charge and discharge, protons rapidly hop among RCOO− sites for oriented transport, fundamentally reducing the effects of electrode tortuosity and polarization resulting from concentration gradients. Consequently, nearly constant ion transport resistance per unit thickness is achieved, even in the case of a 900-μm-thick dense electrode, leading to unprecedented areal capacitances of 14.85 F cm−2 at 1 mA cm−2 and 4.26 F cm−2 at 100 mA cm−2. This study provides an efficient method for accelerating ion transport through thick and dense electrodes, indicating a significant solution for achieving high energy density in energy storage devices, including but not limited to supercapacitors. PubDate: Fri, 14 Jun 2024 00:00:00 GMT DOI: 10.1093/nsr/nwae207 Issue No:Vol. 11, No. 8 (2024)
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First page: nwae199 Abstract: ABSTRACTRechargeable aqueous Zn-ion batteries have been deemed a promising energy storage device. However, the dendrite growth and side reactions have hindered their practical application. Herein, inspired by the ultrafluidic and K+ ion-sieving flux through enzyme-gated potassium channels (KcsA) in biological plasma membranes, a metal-organic-framework (MOF-5) grafted with –ClO4 groups (MOF-ClO4) as functional enzymes is fabricated to mimic the ultrafluidic lipid-bilayer structure for gating Zn2+ ‘on’ and anions ‘off’ states. The MOF-ClO4 achieved perfect Zn2+/SO42− selectivity (∼10), enhanced Zn2+ transfer number (${{t}_{{\rm{Z}}{{{\rm{n}}}^{2 + }}}} = 0.88$) and the ultrafluidic Zn2+ flux (1.9 × 10−3 vs. 1.67 mmol m−2 s−1 for KcsA). The symmetric cells based on MOF-ClO4 achieve a lifespan of over 5400 h at 10 mA cm−2/20 mAh cm−2. Specifically, the performance of the PMCl-Zn//V2O5 pouch cell keeps 81% capacity after 2000 cycles at 1 A g−1. The regulated ion transport, by learning from a biological plasma membrane, opens a new avenue towards ultralong lifespan aqueous batteries. PubDate: Wed, 12 Jun 2024 00:00:00 GMT DOI: 10.1093/nsr/nwae199 Issue No:Vol. 11, No. 8 (2024)
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First page: nwae198 Abstract: We discuss the recent advancement in PDE learning, focusing on Physics Invariant Attention Neural Operator (PIANO). PIANO is a novel neural operator learning framework for deciphering and integrating physical knowledge from PDEs sampled from multi- physical scenarios. PubDate: Thu, 06 Jun 2024 00:00:00 GMT DOI: 10.1093/nsr/nwae198 Issue No:Vol. 11, No. 8 (2024)
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First page: nwae194 Abstract: ABSTRACTSuperconducting infinite-layer (IL) nickelates offer a new platform for investigating the long-standing problem of high-temperature superconductivity. Many models were proposed to understand the superconducting mechanism of nickelates based on the calculated electronic structure, and the multiple Fermi surfaces and multiple orbitals involved create complications and controversial conclusions. Over the past five years, the lack of direct measurements of the electronic structure has hindered the understanding of nickelate superconductors. Here we fill this gap by directly resolving the electronic structures of the parent compound LaNiO2 and superconducting La0.8Ca0.2NiO2 using angle-resolved photoemission spectroscopy. We find that their Fermi surfaces consist of a quasi-2D hole pocket and a 3D electron pocket at the Brillouin zone corner, whose volumes change upon Ca doping. The Fermi surface topology and band dispersion of the hole pocket closely resemble those observed in hole-doped cuprates. However, the cuprate-like band exhibits significantly higher hole doping in superconducting La0.8Ca0.2NiO2 compared to superconducting cuprates, highlighting the disparities in the electronic states of the superconducting phase. Our observations highlight the novel aspects of the IL nickelates, and pave the way toward the microscopic understanding of the IL nickelate family and its superconductivity. PubDate: Tue, 04 Jun 2024 00:00:00 GMT DOI: 10.1093/nsr/nwae194 Issue No:Vol. 11, No. 8 (2024)
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First page: nwae189 Abstract: ABSTRACTA major impediment to the development of the efficient use of artificial photosynthesis is the lack of highly selective and efficient photocatalysts toward the conversion of CO2 by sunlight energy at room temperature and ambient pressure. After many years of hard work, we finally completed the synthesis of graphdiyne-based palladium quantum dot catalysts containing high-density metal atom steps for selective artificial photosynthesis. The well-designed interface structure of the catalyst is composed of electron-donor and acceptor groups, resulting in the obvious incomplete charge-transfer phenomenon between graphdiyne and plasmonic metal nanostructures on the interface. These intrinsic characteristics are the origin of the high performance of the catalyst. Studies on its mechanism reveal that the synergism between ‘hot electron’ from local surface plasmon resonance and rapid photogenerated carrier separation at the ohmic contact interface accelerates the multi-electron reaction kinetics. The catalyst can selectively synthesize CH4 directly from CO2 and H2O with selectivity of near 100% at room temperature and pressure, and exhibits transformative performance, with an average CH4 yield of 26.2 μmol g−1 h−1 and remarkable long-term stability. PubDate: Wed, 29 May 2024 00:00:00 GMT DOI: 10.1093/nsr/nwae189 Issue No:Vol. 11, No. 8 (2024)
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First page: nwae133 Abstract: This paper gives a brief introduction to recent theoretical advance of meta learning. PubDate: Wed, 03 Apr 2024 00:00:00 GMT DOI: 10.1093/nsr/nwae133 Issue No:Vol. 11, No. 8 (2024)
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First page: nwae132 Abstract: ABSTRACTMost optimization problems of practical significance are typically solved by highly configurable parameterized algorithms. To achieve the best performance on a problem instance, a trial-and-error configuration process is required, which is very costly and even prohibitive for problems that are already computationally intensive, e.g. optimization problems associated with machine learning tasks. In the past decades, many studies have been conducted to accelerate the tedious configuration process by learning from a set of training instances. This article refers to these studies as learn to optimize and reviews the progress achieved. PubDate: Tue, 02 Apr 2024 00:00:00 GMT DOI: 10.1093/nsr/nwae132 Issue No:Vol. 11, No. 8 (2024)
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First page: nwae119 Abstract: ABSTRACTArtificial intelligence (AI) tools are changing the way we do science. AlphaFold basically solved the conundrum of protein structure prediction; DeepMD greatly improved the efficiency and accuracy of molecular simulations; and the emerging large language models such as ChatGPT are opening up more possibilities for scientific applications. In this panel, five experts from China and the US discussed the concept, development, bottlenecks and opportunities of AI for Science (AI4S), as well as their understanding of the relationship between AI and science.Roberto CarProfessor at Department of Chemistry, Princeton University, USAWeinan EProfessor at School of Mathematical Sciences, Peking University, China; AI for Science Institute, Beijing, ChinaDavid SrolovitzProfessor at Department of Mechanical Engineering, University of Hong Kong, ChinaHan WangProfessor at the Institute of Applied Physics and Computational Mathematics, Chinese Academy of Sciences, ChinaLinfeng Zhang (Chair)Chief scientific officer of DP Technology, China; AI for Science Institute, Beijing, China PubDate: Tue, 26 Mar 2024 00:00:00 GMT DOI: 10.1093/nsr/nwae119 Issue No:Vol. 11, No. 8 (2024)
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First page: nwae116 Abstract: ABSTRACTFlexible multiplexing chips that permit reconfigurable multidimensional channel utilization are indispensable for revolutionary 6G terahertz communications, but the insufficient manipulation capability of terahertz waves prevents their practical implementation. Herein, we propose the first experimental demonstration of a flexible multiplexing chip for terahertz communication by revealing the unique mechanism of topological phase (TP) transition and perseveration in a heterogeneously coupled bilayer valley Hall topological photonic system. The synthetic and individual TPs operated in the coupled and decoupled states enable controllable on-chip modular TP transitions and subchannel switching. Two time-frequency interleaved subchannels support 10- and 12-Gbit/s QAM-16 high-speed data streams along corresponding paths over carriers of 120 and 130 GHz with 2.5- and 3-GHz bandwidths, respectively. This work unlocks interlayer heterogeneous TPs for inspiring ingenious on-chip terahertz-wave regulation, allowing functionality-reconfigurable, compactly integrated and CMOS-compatible chips. PubDate: Sat, 23 Mar 2024 00:00:00 GMT DOI: 10.1093/nsr/nwae116 Issue No:Vol. 11, No. 8 (2024)
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First page: nwae107 Abstract: ABSTRACTThe magnetic correlations at the superconductor/ferromagnet (S/F) interfaces play a crucial role in realizing dissipation-less spin-based logic and memory technologies, such as triplet-supercurrent spin-valves and ‘π’ Josephson junctions. Here we report the observation of an induced large magnetic moment at high-quality nitride S/F interfaces. Using polarized neutron reflectometry and DC SQUID measurements, we quantitatively determined the magnetization profile of the S/F bilayer and confirmed that the induced magnetic moment in the adjacent superconductor only exists below TC. Interestingly, the direction of the induced moment in the superconductors was unexpectedly parallel to that in the ferromagnet, which contrasts with earlier findings in S/F heterostructures based on metals or oxides. First-principles calculations verified that the unusual interfacial spin texture observed in our study was caused by the Heisenberg direct exchange coupling with constant J∼4.28 meV through d-orbital overlapping and severe charge transfer across the interfaces. Our work establishes an incisive experimental probe for understanding the magnetic proximity behavior at S/F interfaces and provides a prototype epitaxial ‘building block’ for superconducting spintronics. PubDate: Tue, 19 Mar 2024 00:00:00 GMT DOI: 10.1093/nsr/nwae107 Issue No:Vol. 11, No. 8 (2024)
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First page: nwae088 Abstract: This perspective article delves into the transformative realm of dynamic neural networks, which is reshaping AI with adaptable structures and improved efficiency, bridging the gap between artificial and human intelligence. PubDate: Thu, 07 Mar 2024 00:00:00 GMT DOI: 10.1093/nsr/nwae088 Issue No:Vol. 11, No. 8 (2024)
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First page: nwad300 Abstract: Dive into the novel OpenML paradigm, unveiling its transformative approach to robust AI in dynamic environment, shaping Automated Machine Learning with adaptability for ground breaking advancements towards Artificial General Intelligence. PubDate: Tue, 28 Nov 2023 00:00:00 GMT DOI: 10.1093/nsr/nwad300 Issue No:Vol. 11, No. 8 (2023)
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First page: nwad292 Abstract: Formulating the methodology of machine learning by bilevel optimization techniques provides a new perspective to understand and solve automated machine learning problems. PubDate: Tue, 21 Nov 2023 00:00:00 GMT DOI: 10.1093/nsr/nwad292 Issue No:Vol. 11, No. 8 (2023)
Hybrid journal (It can contain Open Access articles)
