A Biphasic Strategy to Synergistically Accelerate Activation and CO Spillover in Formic Acid Oxidation Catalysis

IF 9.6 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Nano Letters Pub Date : 2024-06-20 DOI:10.1021/acs.nanolett.4c02074

Changhong Zhan, Haoran Sun, Wei Yan, Jing Xia, Xiang-Min Meng, Tongtong Li, Lingzheng Bu, Qingyu Kong, Haixin Lin, Wei Liu, Xiaoqing Huang* and Nanjun Chen*,

{"title":"A Biphasic Strategy to Synergistically Accelerate Activation and CO Spillover in Formic Acid Oxidation Catalysis","authors":"Changhong Zhan, Haoran Sun, Wei Yan, Jing Xia, Xiang-Min Meng, Tongtong Li, Lingzheng Bu, Qingyu Kong, Haixin Lin, Wei Liu, Xiaoqing Huang* and Nanjun Chen*, ","doi":"10.1021/acs.nanolett.4c02074","DOIUrl":null,"url":null,"abstract":"Developing highly efficient and carbon monoxide (CO)-tolerant platinum (Pt) catalysts for the formic acid oxidation reaction (FAOR) is vital for direct formic acid fuel cells (DFAFCs), yet it is challenging due to the high energy barrier of direct intermediates (HCOO* and COOH*) as well as the CO poisoning issues associated with Pt alloy catalysts. Here we present a versatile biphasic strategy by creating a hexagonal/cubic crystalline-phase-synergistic PtPb/C (h/c-PtPb/C) catalyst to tackle the aforementioned issues. Detailed investigations reveal that h/c-PtPb/C can simultaneously facilitate the adsorption of direct intermediates while inhibiting CO adsorption, thereby significantly improving the activation and CO spillover. As a result, h/c-PtPb/C showcases an outstanding FAOR activity of 8.1 A mgPt–1, which is 64.5 times higher than that of commercial Pt/C and significantly surpasses monophasic PtPb. Moreover, the h/c-PtPb/C-based membrane electrode assembly exhibits an exceptional peak power density of 258.7 mW cm–2 for practical DFAFC applications.","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":null,"pages":null},"PeriodicalIF":9.6000,"publicationDate":"2024-06-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Nano Letters","FirstCategoryId":"88","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acs.nanolett.4c02074","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}

引用次数: 0

Abstract

Developing highly efficient and carbon monoxide (CO)-tolerant platinum (Pt) catalysts for the formic acid oxidation reaction (FAOR) is vital for direct formic acid fuel cells (DFAFCs), yet it is challenging due to the high energy barrier of direct intermediates (HCOO* and COOH*) as well as the CO poisoning issues associated with Pt alloy catalysts. Here we present a versatile biphasic strategy by creating a hexagonal/cubic crystalline-phase-synergistic PtPb/C (h/c-PtPb/C) catalyst to tackle the aforementioned issues. Detailed investigations reveal that h/c-PtPb/C can simultaneously facilitate the adsorption of direct intermediates while inhibiting CO adsorption, thereby significantly improving the activation and CO spillover. As a result, h/c-PtPb/C showcases an outstanding FAOR activity of 8.1 A mg_Pt^–1, which is 64.5 times higher than that of commercial Pt/C and significantly surpasses monophasic PtPb. Moreover, the h/c-PtPb/C-based membrane electrode assembly exhibits an exceptional peak power density of 258.7 mW cm^–2 for practical DFAFC applications.

查看原文

微信好友朋友圈 QQ好友复制链接

本刊更多论文

在甲酸氧化催化过程中协同加速活化和一氧化碳溢出的双相策略。

为甲酸氧化反应（FAOR）开发高效且耐一氧化碳（CO）的铂（Pt）催化剂对直接甲酸燃料电池（DFAFC）至关重要，但由于直接中间产物（HCOO* 和 COOH*）的高能垒以及与铂合金催化剂相关的 CO 中毒问题，开发这种催化剂具有挑战性。在此，我们通过创建六方/立方晶相协同 PtPb/C（h/c-PtPb/C）催化剂，提出了一种多功能双相策略，以解决上述问题。详细研究表明，h/c-PtPb/C 可在抑制 CO 吸附的同时促进直接中间产物的吸附，从而显著改善活化和 CO 溢出。因此，h/c-PtPb/C 的 FAOR 活性高达 8.1 A mgPt-1，是商用 Pt/C 的 64.5 倍，大大超过了单相 PtPb。此外，基于 h/c-PtPb/C 的膜电极组件的峰值功率密度高达 258.7 mW cm-2，非常适合实际的 DFAFC 应用。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

求助全文

约1分钟内获得全文去求助

来源期刊

Nano Letters 工程技术-材料科学：综合

CiteScore

16.80

自引率

2.80%

发文量

1182

审稿时长

1.4 months

期刊介绍： Nano Letters serves as a dynamic platform for promptly disseminating original results in fundamental, applied, and emerging research across all facets of nanoscience and nanotechnology. A pivotal criterion for inclusion within Nano Letters is the convergence of at least two different areas or disciplines, ensuring a rich interdisciplinary scope. The journal is dedicated to fostering exploration in diverse areas, including: - Experimental and theoretical findings on physical, chemical, and biological phenomena at the nanoscale - Synthesis, characterization, and processing of organic, inorganic, polymer, and hybrid nanomaterials through physical, chemical, and biological methodologies - Modeling and simulation of synthetic, assembly, and interaction processes - Realization of integrated nanostructures and nano-engineered devices exhibiting advanced performance - Applications of nanoscale materials in living and environmental systems Nano Letters is committed to advancing and showcasing groundbreaking research that intersects various domains, fostering innovation and collaboration in the ever-evolving field of nanoscience and nanotechnology.