Ultrasmall palladium nanoparticles supported on zirconium phosphate for electrochemical CO2 reduction to ethanol

IF 6.2 4区 工程技术 Q3 ENERGY & FUELS
Bowen Zhong, Chengwei Hu, Kaian Sun, Wei Yan, Jiujun Zhang, Zailai Xie
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引用次数: 0

Abstract

The electrochemical CO2 reduction reaction (CO2RR) provides a promising approach to mitigate the global greenhouse effect by converting CO2 into high-value chemicals or fuels. Noble metal-based nanomaterials are widely regarded as efficient catalysts for CO2RR due to their high catalytic activity and excellent stability. However, these catalysts typically favor the formation of C1 products, which have relatively low economic value. Moreover, the high cost and limited availability of noble materials necessitate strategies to reduce their usage, often by dispersing them on suitable support materials to enhance catalytic performance. In this study, a novel metal-based support, zirconium phosphate Zr3(PO4)4, was used to anchor ultrasmall palladium nanoparticles (pre-ZrP-Pd). Compared to the reversible hydrogen electrode, the pre-ZrP-Pd achieved a maximum Faradaic efficiency (FE) of 92.1% for ethanol at −0.8 V versus RHE, along with a peak ethanol current density of 0.82 mA/cm2. Density functional theory (DFT) calculations revealed that the strong metal-support interactions between the ZrP support and Pd nanoparticles lead to an upward shift of the Pd d-band center, enhancing the adsorption of CO* and promoting the coupling of CO and CO to produce ethanol.

磷酸锆负载的超小钯纳米颗粒电化学CO2还原为乙醇
电化学二氧化碳还原反应(CO2RR)通过将二氧化碳转化为高价值的化学品或燃料,为减轻全球温室效应提供了一种有前途的方法。贵金属基纳米材料因其高的催化活性和优异的稳定性被广泛认为是高效的CO2RR催化剂。然而,这些催化剂通常有利于形成C1产物,其经济价值相对较低。此外,贵重材料的高成本和有限的可用性需要减少其使用的策略,通常是通过将它们分散在合适的支持材料上以提高催化性能。在这项研究中,一种新型金属基载体磷酸锆Zr3(PO4)4被用于锚定超小钯纳米颗粒(pre-ZrP-Pd)。与可逆氢电极相比,pre-ZrP-Pd在−0.8 V下对乙醇的最大法拉第效率(FE)为92.1%,乙醇的峰值电流密度为0.82 mA/cm2。密度泛函理论(DFT)计算表明,ZrP载体与Pd纳米颗粒之间的强金属-载体相互作用导致Pd -能带中心向上移动,增强了CO*的吸附,促进了CO与CO的偶联生成乙醇。
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来源期刊
Frontiers in Energy
Frontiers in Energy Energy-Energy Engineering and Power Technology
CiteScore
5.90
自引率
6.90%
发文量
708
期刊介绍: Frontiers in Energy, an interdisciplinary and peer-reviewed international journal launched in January 2007, seeks to provide a rapid and unique platform for reporting the most advanced research on energy technology and strategic thinking in order to promote timely communication between researchers, scientists, engineers, and policy makers in the field of energy. Frontiers in Energy aims to be a leading peer-reviewed platform and an authoritative source of information for analyses, reviews and evaluations in energy engineering and research, with a strong focus on energy analysis, energy modelling and prediction, integrated energy systems, energy conversion and conservation, energy planning and energy on economic and policy issues. Frontiers in Energy publishes state-of-the-art review articles, original research papers and short communications by individual researchers or research groups. It is strictly peer-reviewed and accepts only original submissions in English. The scope of the journal is broad and covers all latest focus in current energy research. High-quality papers are solicited in, but are not limited to the following areas: -Fundamental energy science -Energy technology, including energy generation, conversion, storage, renewables, transport, urban design and building efficiency -Energy and the environment, including pollution control, energy efficiency and climate change -Energy economics, strategy and policy -Emerging energy issue
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