Expanding the Environmental Frontiers of Operando Metrology for Advanced Device Materials Development

扩大先进设备材料开发操作计量的环境前沿

• 批准号: EP/T001038/1
• 负责人: Stephan Hofmann
• 金额: $ 130.81万
• 依托单位: University of Cambridge
• 依托单位国家: 英国
• 项目类别: Research Grant
• 财政年份: 2020
• 资助国家: 英国
• 起止时间: 2020 至 无数据
• 项目状态: 已结题
• 来源: https://gtr.ukri.org/projects?ref=EP%2FT001038%2F1
• 关键词: Expanding; Environmental; Frontiers; Operando; Metrology

Lord Kelvin famously stated "when you cannot measure it, when you cannot express it in numbers, your knowledge is of a meagre and unsatisfactory kind". This holds none more true than for nanotechnology today. Emergent materials such as 2D transition metal dichalcogenide (TMD) compounds offer exciting, wide opportunities from novel (opto-) electronic devices to energy storage and catalytic energy conversion. For the latter, TMDs materials like MoS2 have shown high catalytic activity and offer large potential as earth abundant electro-catalysts to for instance convert waste CO2 into industrially relevant chemicals/fuels and to generate hydrogen sustainably, i.e. processes of utmost significance as strategies for a sustainable, clean future economy. However, TMD catalysts can undergo significant chemical and structural changes during reactions, and the mechanisms that give the high catalytic activity remain largely unknown. Our knowledge is currently equally meagre in terms of materials synthesis. There is very little understanding how TMDs actually grow and hence how the structure and properties of these materials can be scalably controlled. These challenges and lack of understanding are common to numerous emerging materials. One key reason for this is that they typically can only be resolved and adequately characterised at a "post-mortem" stage, and we are left to speculate what mechanisms actually govern growth or material functionality at industrially relevant "real-world" conditions.This proposal aims at true operando characterisation of novel materials like TMDs under industrially relevant reactive atmospheres at elevated temperatures, to have a transformative impact on their future use by developing a fundamental understanding of their design and functionality. Our focus will be on electron microscopy and spectroscopy, in particular scanning electron microscopy and X-ray photoelectron spectroscopy, which are among the most wide-spread and versatile characterisation techniques in modern science, used across all disciplines in academia and industry. They are endowed with high (near-)surface sensitivity, making them powerful tools for analysing the structure and chemistry of surfaces and interfaces. However, low-energy electrons are also strongly scattered by gas molecules, and therefore all these techniques are conventionally performed under high vacuum or restricted environmental conditions. We propose new environmental cell approaches that can be flexibly implemented for the many electron-based techniques to overcome these restrictions, and enable direct characterisation at high spatial and/or chemical resolution across an unprecedented range of industrially relevant process conditions for temperatures as high as 1000C and in reactive gaseous or liquid environments. The proposal builds on recent strategic equipment investment at Manchester, Cambridge and the Diamond Light Source/Harwell, and together with market-leading industrial partners our vision is to pioneer versatile approaches that open up new correlative, multi-modal operando probing capability applicable to a wide range of fields including organic semiconductors, battery/energy research, catalysis and life sciences. This will also link to simulation and theory to achieve new levels of understanding and predictive power. Applied to TMD materials, this capability will allow us to directly interrogate TMD nucleation and growth at industrially relevant reactor conditions, to develop new manufacturing processes including for so far largely unexplored metallic compounds. This will further allow us for the first time to systematically study model TMD catalysts under reaction conditions. In particular, we propose to explore metallic TMDs like NbS2, as unlike to semiconducting MoS2, their catalytic activity could extend over the entire basal plane, opening new directions to design novel electro-catalysts with low overpotential and high current densities.

开尔文勋爵曾说过一句名言：“当你无法衡量它，当你无法用数字表达它时，你的知识是贫乏和不令人满意的。对于今天的纳米技术来说，这一点再正确不过了。新兴材料，如2D过渡金属二硫属化物（TMD）化合物提供了令人兴奋的，广泛的机会，从新型（光）电子器件到能量存储和催化能量转换。对于后者，像MoS 2这样的TMD材料已经显示出高催化活性，并作为地球丰富的电催化剂提供了巨大的潜力，例如将废CO2转化为工业相关的化学品/燃料，并可持续地产生氢气，即作为可持续的清洁未来经济战略的最重要的过程。然而，TMD催化剂在反应过程中会发生显着的化学和结构变化，并且提供高催化活性的机制在很大程度上仍然未知。我们的知识目前在材料合成方面同样贫乏。人们对TMD实际上是如何生长的，以及如何可扩展地控制这些材料的结构和性能知之甚少。这些挑战和缺乏理解是许多新兴材料的共同点。其中一个关键原因是，它们通常只能在“事后”阶段被解决和充分表征，并且我们只能推测在工业相关的“真实世界”条件下实际上控制生长或材料功能的机制。该提案旨在在工业相关的反应气氛下在高温下对新型材料如TMD进行真正的操作表征，通过发展对其设计和功能的基本理解，对未来的使用产生变革性影响。我们的重点将是电子显微镜和光谱学，特别是扫描电子显微镜和X射线光电子能谱，这是现代科学中最广泛和最通用的表征技术之一，用于学术界和工业界的所有学科。它们具有高（近）表面灵敏度，使其成为分析表面和界面结构和化学的强大工具。然而，低能电子也被气体分子强烈散射，因此所有这些技术通常在高真空或受限的环境条件下进行。我们提出了新的环境电池方法，可以灵活地实现许多基于电子的技术，以克服这些限制，并使直接表征在高空间和/或化学分辨率在前所未有的范围内的工业相关的工艺条件的温度高达1000 ℃和反应气体或液体环境。该提案建立在最近在曼彻斯特，剑桥和钻石光源/哈威尔的战略设备投资的基础上，并与市场领先的工业合作伙伴一起，我们的愿景是开创多功能方法，开辟新的相关，多模态操作探测能力，适用于广泛的领域，包括有机半导体，电池/能源研究，催化和生命科学。这也将与模拟和理论联系起来，以实现新的理解和预测能力。应用于TMD材料，这种能力将使我们能够在工业相关的反应器条件下直接询问TMD成核和生长，以开发新的制造工艺，包括迄今为止尚未开发的金属化合物。这将进一步使我们第一次系统地研究模型TMD催化剂的反应条件。特别是，我们建议探索金属TMD，如NbS 2，与半导体MoS 2不同，它们的催化活性可以延伸到整个基面，为设计具有低过电位和高电流密度的新型电催化剂开辟了新的方向。

项目成果

Empirical Parameter to Compare Molecule-Electrode Interfaces in Large-Area Molecular Junctions.

• DOI: 10.1021/acsphyschemau.1c00029
• 发表时间: 2022-05-25
• 期刊: ACS PHYSICAL CHEMISTRY AU
• 作者: Carlotti, Marco;Soni, Saurabh;Kovalchuk, Andrii;Kumar, Sumit;Hofmann, Stephan;Chiechi, Ryan C
• 通讯作者: Chiechi, Ryan C

Crystal Orientation Dependent Oxidation Modes at the Buried Graphene-Cu Interface.

• DOI: 10.1021/acs.chemmater.0c02296
• 发表时间: 2020-09-22
• 期刊: Chemistry of materials : a publication of the American Chemical Society
• 作者: Braeuninger-Weimer P;Burton OJ;Zeller P;Amati M;Gregoratti L;Weatherup RS;Hofmann S
• 通讯作者: Hofmann S

Electron beam evaporation of superconductor-ferromagnet heterostructures.

• DOI: 10.1038/s41598-022-11828-y
• 发表时间: 2022-05-11
• 期刊: Scientific reports
• 影响因子: 4.6

Putting High-Index Cu on the Map for High-Yield, Dry-Transferred CVD Graphene.

将高索引Cu放在地图上，以进行高收益，干燥的CVD石墨烯。

• DOI: 10.1021/acsnano.2c09253
• 发表时间: 2023-01-03
• 期刊: ACS NANO
• 影响因子: 17.1
• 作者: Burton, Oliver J.;Winter, Zachary;Watanabe, Kenji;Taniguchi, Takashi;Beschoten, Bernd;Stampfer, Christoph;Hofmann, Stephan
• 通讯作者: Hofmann, Stephan

Putting high-index Cu on the map for high-yield, dry-transferred CVD graphene

将高指数 Cu 应用于高产干转移 CVD 石墨烯

• DOI: 10.48550/arxiv.2209.08007
• 发表时间: 2022
• 作者: Burton O