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ArticleCathodic Corrosion-Induced Structural Evolution of CuNi Electrocatalysts for Enhanced CO2 ReductionWenjin Sun 1,†, Bokki Min 2,†, Maoyu Wang 3, Xue Han 4, Qiang Gao 1, Sooyeon Hwang 5, Hua Zhou 3, and Huiyuan Zhu 1,2,*1 Department of Chemistry, University of Virginia, Charlottesville, VA 22904, USA2 Department of Chemical Engineering, University of Virginia, Charlottesville, VA 22904, USA3 Advanced Photon Source, Argonne National Laboratory, Lemont, IL 60439, USA4 Department of Chemical Engineering, Virginia Polytechnic Institute and State University, Blacksburg, VA 24061, USA5 Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, NY 11973, USA* Correspondence: kkx8js@virginia.com† These authors contributed equally to this work.Received: 22 October 2024; Revised: 25 November 2024; Accepted: 27 November 2024; Published: 4 December 2024 Abstract: The electrochemical CO2 reduction reaction (CO2RR) has attracted significant attention as a promising strategy for storing intermittent energy in chemical bonds while sustainably producing value-added chemicals and fuels. Copper-based bimetallic catalysts are particularly appealing for CO2RR due to their unique ability to generate multi-carbon products. While substantial effort has been devoted to developing new catalysts, the evolution of bimetallic systems under operational conditions remains underexplored. In this work, we synthesized a series of CuxNi1−x nanoparticles and investigated their structural evolution during CO2RR. Due to the higher oxophilicity of Ni compared to Cu, the particles tend to become Ni-enriched at the surface upon air exposure, promoting the competing hydrogen evolution reaction (HER). At negative activation potentials, cathodic corrosion has been observed in CuxNi1−x nanoparticles, leading to the significant Ni loss and the formation of irregularly shaped Cu nanoparticles with increased defects. This structural evolution, driven by cathodic corrosion, shifts the electrolysis from HER toward CO2 reduction, significantly enhancing the Faradaic efficiency of multi-carbon products (C2+). 

Fine-grained urban flow inference (FUFI), which involves inferring fine-grained flow maps from their coarse-grained counterparts, is of tremendous interest in the realm of sustainable urban traffic services. To address the FUFI, existing solutions mainly concentrate on investigating spatial dependencies, introducing external factors, reducing excessive memory costs, etc., -- while rarely considering the catastrophic forgetting (CF) problem. Motivated by recent operator learning, we present an Urban Neural Operator solution with Incremental learning (UNOI), primarily seeking to learn grained-invariant solutions for FUFI in addition to addressing CF. Specifically, we devise an urban neural operator (UNO) in UNOI that learns mappings between approximation spaces by treating the different-grained flows as continuous functions, allowing a more flexible capture of spatial correlations. Furthermore, the phenomenon of CF behind time-related flows could hinder the capture of flow dynamics. Thus, UNOI mitigates CF concerns as well as privacy issues by placing UNO blocks in two incremental settings, i.e., flow-related and task-related. Experimental results on large-scale real-world datasets demonstrate the superiority of our proposed solution against the baselines. 

Understanding human mobility has become an important aspect of location-based services in tasks such as personalized recommendation and individual moving pattern recognition, enabled by the large volumes of data from geo-tagged social media (GTSM). Prior studies mainly focus on analyzing human historical footprints collected by GTSM and assuming the veracity of the data, which need not hold when some users are not willing to share their real footprints due to privacy concerns—thereby affecting reliability/authenticity. In this study, we address the problem of Inferring Real Mobility (IRMo) of users, from their unreliable historical traces. Tackling IRMo is a non-trivial task due to the: (1) sparsity of check-in data; (2) suspicious counterfeit check-in behaviors; and (3) unobserved dependencies in human trajectories. To address these issues, we develop a novel Graph-enhanced Attention model calledIRMoGA, which attempts to capture underlying mobility patterns and check-in correlations by exploiting the unreliable spatio-temporal data. Specifically, we incorporate the attention mechanism (rather than solely relying on traditional recursive models) to understand the regularity of human mobility, while employing a graph neural network to understand the mutual interactions from human historical check-ins and leveraging prior knowledge to alleviate the inferring bias. Our experiments conducted on four real-world datasets demonstrate the superior performance of IRMoGA over several state-of-the-art baselines, e.g., up to 39.16% improvement regarding the Recall score on Foursquare. 

The indirect exchange interaction between local magnetic moments via surface electrons has been long predicted to bolster the surface ferromagnetism in magnetic topological insulators (MTIs), which facilitates the quantum anomalous Hall effect. This unconventional effect is critical to determining the operating temperatures of future topotronic devices. However, the experimental confirmation of this mechanism remains elusive, especially in intrinsic MTIs. Here, we combine time-resolved photoemission spectroscopy with time-resolved magneto-optical Kerr effect measurements to elucidate the unique electromagnetism at the surface of an intrinsic MTI MnBi₂Te₄. Theoretical modeling based on 2D Ruderman-Kittel-Kasuya-Yosida interactions captures the initial quenching of a surface-rooted exchange gap within a factor of two but overestimates the bulk demagnetization by one order of magnitude. This mechanism directly explains the sizable gap in the quasi-2D electronic state and the nonzero residual magnetization in even-layer MnBi₂Te₄. Furthermore, it leads to efficient light-induced demagnetization comparable to state-of-the-art magnetophotonic crystals, promising an effective manipulation of magnetism and topological orders for future topotronics. 

Typically, trajectories considered anomalous are the ones deviating from usual (e.g., traffic-dictated) driving patterns. However, this closed-set context fails to recognize the unknown anomalous trajectories, resulting in an insufficient self-motivated learning paradigm. In this study, we investigate the novel Anomalous Trajectory Recognition problem in an Open-world scenario (ATRO) and introduce a novel probabilistic Metric learning model, namely ATROM, to address it. Specifically, ATROM can detect the presence of unknown anomalous behavior in addition to identifying known behavior. It has a Mutual Interaction Distillation that uses contrastive metric learning to explore the interactive semantics regarding the diverse behavioral intents and a Probabilistic Trajectory Embedding that forces the trajectories with distinct behaviors to follow different Gaussian priors. More importantly, ATROM offers a probabilistic metric rule to discriminate between known and unknown behavioral patterns by taking advantage of the approximation of multiple priors. Experimental results on two large-scale trajectory datasets demonstrate the superiority of ATROM in addressing both known and unknown anomalous patterns.