PtRu Intra-Cluster Electron Modulation Accelerates Multi-Scenario Hydrogen Evolution Reaction

IF 24.4 1区 材料科学 Q1 CHEMISTRY, PHYSICAL
Xue Zhao, Yaling Jiang, Dan Wang, Yicheng Zhang, Mengshan Chen, Guangzhi Hu, Haibo Zhang, Zhong Jin, Yingtang Zhou
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引用次数: 0

Abstract

The development of advanced nanomaterial manufacturing technology and the in-depth analysis of the structure-activity relationship are conducive to the sustainable development of platinum-based catalysts in terms of low cost and high performance. The in situ conversion of Pt4+ and Ru3+ is creatively achieved into highly dispersed, small-sized heterojunction clusters in the confined space by reductant preset framework materials, and these clusters benefited from the hollow carbon spheres gap supramolecular self-assembly strategy to achieve high exposure. The intra-cluster Ru→Pt electron transfer and induced electronic structure modulation enhance the adsorption and activation of H2O molecules at the interface, accelerating the desorption coupling of [H] at the Pt or Ru site. As a catalyst, PtRu/BNHCSs have achieved significant hydrogen production from electrolyzed water in multiple scenarios, exceeding the performance of the commercial Pt/C catalyst. These scenarios include high-current water splitting to hydrogen in both pH-neutral and simulated seawater, direct seawater hydrogen production, and anion-exchange membrane integrated continuous and efficient electrolytic hydrogen production. In situ Fourier transform infrared and in situ Raman interface monitoring techniques reveal the interfacial adsorption behavior of H2O, providing important experimental and theoretical insights for understanding and revealing the synergistic effect and the interfacial reaction behavior of intra-cluster atoms of PtRu heterojunction.

Abstract Image

PtRu簇内电子调制加速多场景析氢反应
先进纳米材料制造技术的发展和对其构效关系的深入分析,有利于铂基催化剂在低成本、高性能方面的可持续发展。通过还原剂预设的框架材料,创造性地实现了Pt4+和Ru3+在密闭空间内的原位转化成高度分散的小尺寸异质结团簇,这些团簇得益于中空碳球间隙超分子自组装策略实现了高曝光。簇内Ru→Pt电子转移和诱导的电子结构调制增强了界面处H2O分子的吸附和活化,加速了[H]在Pt或Ru位点的脱附耦合。作为催化剂,PtRu/ bnhcs在多种情况下从电解水中获得了显著的制氢效果,超过了商用Pt/C催化剂的性能。这些场景包括在ph中性和模拟海水中大电流水裂解制氢、海水直接制氢和阴离子交换膜集成连续高效电解制氢。原位傅立叶变换红外和原位拉曼界面监测技术揭示了水的界面吸附行为,为理解和揭示PtRu异质结簇内原子的协同效应和界面反应行为提供了重要的实验和理论见解。
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来源期刊
Advanced Energy Materials
Advanced Energy Materials CHEMISTRY, PHYSICAL-ENERGY & FUELS
CiteScore
41.90
自引率
4.00%
发文量
889
审稿时长
1.4 months
期刊介绍: Established in 2011, Advanced Energy Materials is an international, interdisciplinary, English-language journal that focuses on materials used in energy harvesting, conversion, and storage. It is regarded as a top-quality journal alongside Advanced Materials, Advanced Functional Materials, and Small. With a 2022 Impact Factor of 27.8, Advanced Energy Materials is considered a prime source for the best energy-related research. The journal covers a wide range of topics in energy-related research, including organic and inorganic photovoltaics, batteries and supercapacitors, fuel cells, hydrogen generation and storage, thermoelectrics, water splitting and photocatalysis, solar fuels and thermosolar power, magnetocalorics, and piezoelectronics. The readership of Advanced Energy Materials includes materials scientists, chemists, physicists, and engineers in both academia and industry. The journal is indexed in various databases and collections, such as Advanced Technologies & Aerospace Database, FIZ Karlsruhe, INSPEC (IET), Science Citation Index Expanded, Technology Collection, and Web of Science, among others.
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