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.

该项目将研究金属催化剂上的电化学催化，这些催化剂完全或部分被超薄多孔材料层覆盖。 将评估涂层催化剂在促进与燃料电池有关的清洁能源技术和减少二氧化碳排放方面的有效性。 这项研究将与教学和外联工作相结合，强调众包工具和基于问题的学习原则，积极吸引学生和公民科学家参与创新清洁能源技术的开发和评估。该项目将专注于定义明确的平面电极，其上将通过室温紫外线（UV）-臭氧工艺沉积氧化硅和氧化钛的超薄覆盖层，该工艺允许对氧化物厚度进行纳米级控制。 氧化物膜的厚度和表面化学性质将被调整以控制活性物质的选择性传输和/或修改掩埋界面处的独特催化位点。定义明确的氧化物封装的电催化剂将使用一套成像和光谱技术，将能够i.）输运和动力学效应的解卷积，ii.）阐明氧化物覆盖层影响反应选择性的机制，和iii.）设计规则的发展，可适用于广泛的材料和反应。实验测量将与合作者进行的数值模拟和密度泛函理论计算密切协调。本研究的一个具体重点是比较掩埋氧化物/金属界面的氧化物/金属/电解质三相边界网站的催化性能。总体而言，拟议的研究将奠定基础的合理设计的稳定的氧化物封装的电催化剂能够高效和选择性的发电和使用的燃料。 除了具体的研究之外，该项目还将启动一项名为“众包能源创新”的倡议，该倡议将利用新兴的众包原则和在线工具，加速培养今天的学生成为明天能源技术的发明者和评估者，二）增加对国家创新网络的参与，以及iii.）提高学生和公众对尖端清洁能源技术的认识。该奖项反映了NSF的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准进行评估，被认为值得支持。

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.