Exploring Pulsed Laser Ablation in Liquids as a New Synthetic Path Toward Electrocatalysts

本研究将探讨一种新的技术，脉冲激光烧蚀液体（PLAL）用于制备纳米电催化剂。PLAL是一种很有前途的合成方法，用于制备纳米颗粒，不需要有毒化学品，并且易于扩展-有利于未来的发展。PLAL实际上被视为一种最大限度地减少化学品使用的技术，是一种非常“绿色”的技术。 在这项提案中，将在二氧化碳（CO2）电化学转化为有用产品（如甲酸盐，乙醇等）的过程中对PLAL生成的纳米颗粒电催化剂进行研究。政府间气候变化专门委员会最近的一份2018年报告清楚地表明，需要新的解决方案来成功解决日益严重的全球变暖和二氧化碳排放问题。然而，二氧化碳是一种非常稳定的分子。因此，需要电催化剂，即降低反应能量需求的材料来转化CO2。该研究计划的一个方面是制备这样的电催化剂。PLAL将首先用于合成monohydrin纳米粒子，以验证我们的合成方法对当前的电催化剂。然后，从容易获得的材料（如锡或镍）中制备双金属纳米颗粒，并用于CO2电解槽，这是一种利用电力将CO2转化为其他化学品的装置。类似于电池，电解槽有两极，或者正式地说，有两个电极。本研究计划的第二个方面是第二电极的研究。目前，在该第二电极处发生的反应是水氧化成氧--一种在市售碱性电解槽中用于从水中产生氢气和氧气的环境友好反应。然而，CO2电解槽不像碱性水电解槽那样在相同的实验条件下运行，因此重新评估适合转化CO2的催化剂的选择至关重要。 该提议的最后一个非常有吸引力的方面是新型电解槽的设计，该电解槽在一个电极处将CO2消除与在另一个电极处的另一种废物产物（例如肼或尿素）的转化相结合。这种包容性设计还可以减少转化二氧化碳所需的能量。由于PLAL是一种多功能的技术，它将允许合成纳米材料，以探索所描述的各个方面。最终，这项研究计划与环境相关，因为使用这种方法制备电催化剂将有助于缓解气候变化，并缓解我们向可再生能源的过渡。此外，PLAL方法最大限度地减少了有毒化学品的使用，并且易于扩大规模，从而为二氧化碳排放的紧迫环境问题提供了可持续的解决方案。从长远来看，该计划可以为更广泛地使用PLAL铺平道路，例如解决与电池材料或燃料电池相关的挑战。

This proposal will investigate the use of a novel technique, pulsed laser ablation in liquids (PLAL) for preparing nanoparticle electrocatalysts. PLAL is a promising synthetic approach for preparing nanoparticles that does not require toxic chemicals and is easily scable - advantageous for future developments. PLAL is actually viewed as a technique that minimizes chemical use, making a very "green" technique. In this proposal, PLAL-generated nanoparticle electrocatalysts will be examined in the electrochemical conversion of carbon dioxide (CO2) to useful products, such as formate salts, ethanol, etc. A recent, 2018 report from the Intergovernmental Panel on Climate Change clearly demonstrates that new solutions are needed to successfully tackle the growing problem of global warming and CO2 emissions. However, CO2 is a very stable molecule. Thus, electrocatalysts, materials that reduce the energy requirements for a reaction, are required convert CO2. One aspect of this research program is to prepare such electrocatalysts. PLAL will first be used to synthesize monometallic nanoparticles to validate our synthetic approach against current electrocatalysts. Bimetallic nanoparticles from readily available materials, such as tin or nickel, will then be prepared and employed in a CO2 electrolyzer, a device that converts CO2 into other chemicals, using electricity. Akin to a battery, an electrolyzer has two poles or, formally speaking, two electrodes. The second aspect of this research program is the study of the second electrode. Currently, the reaction occurring at this second electrode is the water oxidation to oxygen - an environmentally friendly reaction used in commercially-available alkaline electrolyzers to generate hydrogen and oxygen from water. However, CO2 electrolyzers do not operate under the same experimental conditions as alkaline water electrolyzers, therefore it is critical to reevaluate the choice of catalysts appropriate to convert CO2. The last, and very attractive, aspect of this proposal is the design of novel electrolyzers that incorporate CO2 elimination at one electrode with the conversion of another waste product, such as hydrazine or urea, at the other electrode. Such an inclusive design may also decrease the energy required to convert CO2. As PLAL is a versatile technique, it will allow the synthesis of nanomaterials for exploring all aspects described. Ultimately, this research program is environmentally relevant, as preparing electrocatalysts using this approach will help mitigate climate change and ease our transition toward renewable energies. Furthermore, the PLAL approach minimizes the use of toxic chemicals and is easy to scale up, thereby offering a sustainable solution to the pressing environmental problem of CO2 emissions. In long term, this program could pave the way toward a broader use of PLAL, for example to tackle challenges associated with battery materials or fuel cells.