CAREER: SusChEM: Tunable Electrocatalysis at Buried Interfaces

职业：SusChEM：埋地界面的可调电催化

• 批准号: 1752340
• 负责人: Daniel Esposito
• 金额: $ 58.65万
• 依托单位: Columbia University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2018
• 资助国家: 美国
• 起止时间: 2018-03-15 至 2023-12-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1752340&HistoricalAwards=false
• 关键词: CAREER; SusChEM; Tunable; Electrocatalysis; Buried

The project will investigate electrochemical catalysis on metal catalysts that are fully- or partially-covered by ultra-thin layers of porous materials. The coated catalysts will be evaluated for their effectiveness in promoting clean energy technologies related to fuel cells and reduction of carbon dioxide emissions. The research will be coupled with teaching and outreach efforts emphasizing crowdsourcing tools and problem-based learning principles that actively engage students and citizen scientists in the generation and evaluation of innovative clean energy technologies. The project will focus on well-defined planar electrodes on which ultra-thin overlayers of silicon oxide and titanium oxide will be deposited by a room temperature ultraviolet (UV)- Ozone process that allows for nanometer-level control of the oxide thickness. The thickness and surface chemistry of the oxide films will be tuned to control the selective transport of active species and/or modify the unique catalytic sites at the buried interface. The well-defined oxide-encapsulated electrocatalysts will be investigated for alcohol oxidation and carbon dioxide reduction using a suite of imaging and spectroscopy techniques that will enable i.) deconvolution of transport and kinetic effects, ii.) elucidation of the mechanisms by which ultrathin oxide overlayers influence reaction selectivity, and iii.) the development of design rules that can be applied across a wide range of materials and reactions. Experimental measurements will be closely coordinated with numerical modeling and density functional theory calculations performed by collaborators. A specific focus of this research is to compare the catalytic properties of buried oxide/metal interfaces to those at oxide/metal/electrolyte triple-phase boundary sites. Overall, the proposed research will lay the groundwork for the rational design of stable oxide-encapsulated electrocatalysts capable of highly efficient and selective generation and use of fuels. Beyond the specific research, the project will launch an initiative entitled "Crowdsourcing for Energy Innovation" that will leverage emerging crowdsourcing principles and online tools to i.) accelerate training of today's students to become the inventors and evaluators of tomorrow's energy technology, ii.) increase participation in the Nation's innovation network, and iii.) increase student and public awareness of cutting-edge clean energy technologies.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.

该项目将研究由超薄多孔材料完全或部分覆盖的金属催化剂上的电化学催化。 将评估涂层催化剂在促进与燃料电池相关的清洁能源技术和二氧化碳排放量减少方面的有效性。 这项研究将与教学和外展工作相结合，强调众包工具和基于问题的学习原理，这些学习原理积极吸引学生和公民科学家参与创新的清洁能源技术的一代和评估。该项目将集中在定义明确的平面电极上，氧化硅和氧化钛的超薄叠加剂将通过室温紫外线（UV） - 臭氧工艺沉积，该过程允许对氧化物厚度的纳米水平控制。 氧化物膜的厚度和表面化学将被调整以控制活性物种的选择性运输和/或修改埋入界面处的独特催化位点。将研究使用成像和光谱技术的套件来研究良好定义的氧化物封装电催化剂，以进行酒精氧化和二氧化碳的还原，从而使运输和动力学效应的反趋化效果，II。），II。ii。），将氧化物覆盖的机制逐渐覆盖了综合材料的范围，并且可以跨越了Apprientive Apprientive Apprientive and in III和III II的发展。反应。实验测量将与合作者执行的数值建模和密度功能理论计算密切协调。这项研究的一个特定重点是将掩埋的氧化物/金属界面的催化特性与氧化物/金属/电解质三相边界部位的催化特性进行比较。总体而言，拟议的研究将为能够高效且选择性地产生和使用燃料的稳定的氧化封闭电催化剂的合理设计奠定基础。 除具体研究之外，该项目还将发起一项题为“能源创新众包”的计划，该计划将利用新兴的众包原则和在线工具向i。法定任务，并被认为是值得通过基金会的智力优点和更广泛影响的审查标准来评估的值得支持的。

项目成果

Ultrathin Silicon Oxide Overlayers Enable Selective Oxygen Evolution from Acidic and Unbuffered pH-Neutral Seawater

• DOI: 10.1021/acscatal.0c04343
• 发表时间: 2021-01-12
• 期刊: ACS CATALYSIS
• 影响因子: 12.9
• 作者: Bhardwaj, Amar A.;Vos, Johannes G.;Esposito, Daniel, V
• 通讯作者: Esposito, Daniel, V

Silicon Oxide-Encapsulated Platinum Thin Films as Highly Active Electrocatalysts for Carbon Monoxide and Methanol Oxidation

• DOI: 10.1021/acscatal.8b03626
• 发表时间: 2018-10
• 期刊: ACS Catalysis
• 影响因子: 12.9
• 作者: Jacob Robinson;N. Labrador;Han Chen;B. E. Sartor;D. Esposito

Controlling the Relative Fluxes of Protons and Oxygen to Electrocatalytic Buried Interfaces with Tunable Silicon Oxide Overlayers

使用可调二氧化硅覆盖层控制电催化埋入界面的质子和氧气的相对通量

• DOI: 10.1021/acsaem.0c02359
• 发表时间: 2020
• 期刊: ACS Applied Energy Materials
• 影响因子: 6.4
• 作者: Beatty, Marissa E.;Gillette, Eleanor I.;Haley, Alexis T.;Esposito, Daniel V.
• 通讯作者: Esposito, Daniel V.