SearcharxivSearch

arXiv subjects

Hengyu Li

Publications and source records attributed to Hengyu Li.

7 recordsLinked to original sources

Exceptional Alkaline Methanol Electrooxidation on Bi-modified Pt3M Intermetallics: Kinetic Origins and an OH Binding Energy Descriptor

The exploration of advanced CO-free catalysts and clarifying the ambiguous kinetic origins and governing factors would undoubtedly open up opportunities to overcome the sluggish kinetics of methanol electrooxidation and promote the development of direct methanol fuel cells. Herein, we constructed a family of Bi-modified Pt3M intermetallic catalysts (Bi-Pt3M/C, M=Cr, Mn, Co, Zn, In, Ga, and Sn) that follow CO-free dominated pathway and exhibit exceptional catalytic activity. More significantly, leveraging this platform, we have identified the pivotal factor governing the reaction kinetics in CO-free pathway, namely OH binding energy (OHBE). This arises because the rate-determining step (RDS) encompasses both C-H bond activation and water dissociation, whose respective barriers can be reflected by the OHBE. Accordingly, OHBE can act as an activity descriptor. Specifically, Bi-Pt3In/C stands out from other Bi-Pt3M/C and delivers the unprecedented mass activity of 36.7 A mgPt-1 at peak potential, far exceeding state-of-the-art Pt-based catalysts reported to date. Taking Bi-Pt3In/C as a proof of concept, we clearly elucidate the origin of enhanced MOR activity by combining theoretical calculations, kinetic isotope effects, and formaldehyde electrooxidation. Moreover, there exhibits a volcano-type trend between OHBE and the activity of Bi-Pt3M/C. Beyond the discovery of ultrahigh-performance catalysts, these findings provide a detailed mechanistic picture of RDS and offer an innovative design principle for advanced catalysts.

physics.chem-ph

Cross-layer Attention Sharing for Pre-trained Large Language Models

To enhance the efficiency of the attention mechanism within large language models (LLMs), previous works primarily compress the KV cache or group attention heads, while largely overlooking redundancy between layers. Our comprehensive analyses across various LLMs show that highly similar attention patterns persist within most layers. It's intuitive to reduce the redundancy by sharing attention weights across layers. However, further analysis reveals two challenges: (1) Directly sharing the weight matrix without carefully rearranging the attention heads proves to be ineffective; (2) Shallow layers are vulnerable to small deviations in attention weights. Driven by these insights, we introduce LISA, a lightweight substitute for self-attention in well-trained LLMs. LISA employs tiny feed-forward networks to align attention heads between adjacent layers and low-rank matrices to approximate differences in layer-wise attention weights. Evaluations encompassing 13 typical benchmarks demonstrate that LISA maintains high response quality in terms of accuracy and perplexity while reducing redundant attention calculations within 53%-84% of the total layers. Our implementations of LISA achieve a 6x compression of Q and K matrices within the attention mechanism, with maximum throughput improvements 19.5%, 32.3%, and 40.1% for LLaMA3-8B, LLaMA2-7B, and LLaMA2-13B, respectively.

cs.CL

Boosting Text-To-Image Generation via Multilingual Prompting in Large Multimodal Models

Previous work on augmenting large multimodal models (LMMs) for text-to-image (T2I) generation has focused on enriching the input space of in-context learning (ICL). This includes providing a few demonstrations and optimizing image descriptions to be more detailed and logical. However, as demand for more complex and flexible image descriptions grows, enhancing comprehension of input text within the ICL paradigm remains a critical yet underexplored area. In this work, we extend this line of research by constructing parallel multilingual prompts aimed at harnessing the multilingual capabilities of LMMs. More specifically, we translate the input text into several languages and provide the models with both the original text and the translations. Experiments on two LMMs across 3 benchmarks show that our method, PMT2I, achieves superior performance in general, compositional, and fine-grained assessments, especially in human preference alignment. Additionally, with its advantage of generating more diverse images, PMT2I significantly outperforms baseline prompts when incorporated with reranking methods. Our code and parallel multilingual data can be found at https://github.com/takagi97/PMT2I.

cs.CL

Unveiling High Selectivity Origin of Pt-Bi Catalysts for Alkaline Methanol Electrooxidation via CO-free pathway

A long-standing puzzle for methanol electrooxidation is how to achieve a CO-free pathway and accurately understand the origin of electrocatalytic selectivity. Herein, we unequivocally demonstrate that the Bi-modified Pt/C follows a CO-free dominated pathway during alkaline methanol electrooxidation, and unveil the formaldehyde (HCHO) intermediate as a critical factor influencing pathway selectivity. These findings are substantiated by kinetic isotope effects, formate Faradaic efficiency, in situ spectroscopy, ab initio molecular dynamic simulations, and density functional theory calculations. Bi modification significantly increases the HCHO dehydrogenation barrier, which facilitates its desorption and subsequent conversion to the H2COOH- anion at the alkaline interface, intrinsically avoiding CO formation. More specifically, the formation of ensemble sites featuring V-shaped Bi-Pt-Bi configuration inhibits the cleavage of C-H bond, and the weak OH binding energy at Bi adatoms effectively prevents blockage of oxygenated species, allowing such ensemble sites to fulfill their functional role. Our study opens up a novel dimension for designing advanced CO-free catalysts.

physics.chem-ph

Refining Self-Supervised Learnt Speech Representation using Brain Activations

It was shown in literature that speech representations extracted by self-supervised pre-trained models exhibit similarities with brain activations of human for speech perception and fine-tuning speech representation models on downstream tasks can further improve the similarity. However, it still remains unclear if this similarity can be used to optimize the pre-trained speech models. In this work, we therefore propose to use the brain activations recorded by fMRI to refine the often-used wav2vec2.0 model by aligning model representations toward human neural responses. Experimental results on SUPERB reveal that this operation is beneficial for several downstream tasks, e.g., speaker verification, automatic speech recognition, intent classification.One can then consider the proposed method as a new alternative to improve self-supervised speech models.

eess.AS

A Novel Method for Extrinsic Calibration of Multiple RGB-D Cameras Using Descriptor-Based Patterns

This letter presents a novel method to estimate the relative poses between RGB-D cameras with minimal overlapping fields of view in a panoramic RGB-D camera system. This calibration problem is relevant to applications such as indoor 3D mapping and robot navigation that can benefit from a 360$^\circ$ field of view using RGB-D cameras. The proposed approach relies on descriptor-based patterns to provide well-matched 2D keypoints in the case of a minimal overlapping field of view between cameras. Integrating the matched 2D keypoints with corresponding depth values, a set of 3D matched keypoints are constructed to calibrate multiple RGB-D cameras. Experiments validated the accuracy and efficiency of the proposed calibration approach, both superior to those of existing methods (800 ms vs. 5 seconds; rotation error of 0.56 degrees vs. 1.6 degrees; and translation error of 1.80 cm vs. 2.5 cm.

eess.IV

Construction of all-in-focus images assisted by depth sensing

Multi-focus image fusion is a technique for obtaining an all-in-focus image in which all objects are in focus to extend the limited depth of field (DoF) of an imaging system. Different from traditional RGB-based methods, this paper presents a new multi-focus image fusion method assisted by depth sensing. In this work, a depth sensor is used together with a color camera to capture images of a scene. A graph-based segmentation algorithm is used to segment the depth map from the depth sensor, and the segmented regions are used to guide a focus algorithm to locate in-focus image blocks from among multi-focus source images to construct the reference all-in-focus image. Five test scenes and six evaluation metrics were used to compare the proposed method and representative state-of-the-art algorithms. Experimental results quantitatively demonstrate that this method outperforms existing methods in both speed and quality (in terms of comprehensive fusion metrics). The generated images can potentially be used as reference all-in-focus images.

cs.CV