Periodic Reporting for period 2 - MOFAmmonia (All Metal-Organic Framework-Based Architecture for Efficient Electrocatalytic Ammonia Production)
Período documentado: 2022-08-01 hasta 2024-01-31
Electrocatalytic N2 reduction reaction (NRR) stands as one of the most promising green alternatives to achieve clean, carbon-free and sustainable ammonia (NH3) production, solving the globe’s future production of food and feed-stock chemicals, and serve as practical carrier of sustainable energy. Despite the significant progress in this field, NRR electrocatalysts exhibiting both high activity and selectivity do not exist today and novel materials are still much sought after. Thus, the development of suitable catalytic materials will be a game changer, allowing NRR to fulfil its role in the globe’s energy-economy landscape. Our research aim is to develop a new concept to combine the virtues of both pristine and converted Metal-Organic Framework (MOF) based materials, forming a new strategy to overcome the activity and selectivity limitations of currently-explored NRR electrocatalytic systems.
From the beginning of the project, our primary focus was on developing novel functional electrocatalysts based on MOF-converted metal-ceramics and pristine MOF-based membranes that are tunable in terms of their thickness and chemical properties. In addition, we put a lot of effort into developing and optimizing the techniques for membrane deposition on top of our working electrodes.
To address these goals, we started with synthesis and post-synthetic modifications of MOF-based membranes that later were controllably applied on the solid electrocatalysts by different techniques. Using one of the most advanced technologies available in our lab, scanning electrochemical microscopy (SECM), we could electro-deposit MOFs on top of various solid electrocatalysts, even on the microscopic level.
Our study of these membranes revealed that we can successfully alter the rate and selectivity of the electrocatalysts. The developed metal-organic framework-based membranes were capable of the reactant’s mass-transport attenuation and stabilization of reaction intermediates, partially due to imposed electrostatic secondary-sphere interactions at the vicinity of the active sites. The boosted performance of the coated electrocatalysts is an essential milestone towards fulfilling our research goals.
To address these goals, we started with synthesis and post-synthetic modifications of MOF-based membranes that later were controllably applied on the solid electrocatalysts by different techniques. Using one of the most advanced technologies available in our lab, scanning electrochemical microscopy (SECM), we could electro-deposit MOFs on top of various solid electrocatalysts, even on the microscopic level.
Our study of these membranes revealed that we can successfully alter the rate and selectivity of the electrocatalysts. The developed metal-organic framework-based membranes were capable of the reactant’s mass-transport attenuation and stabilization of reaction intermediates, partially due to imposed electrostatic secondary-sphere interactions at the vicinity of the active sites. The boosted performance of the coated electrocatalysts is an essential milestone towards fulfilling our research goals.
The most exciting breakthrough so far was achieved in a study of a MOF-based membrane used for CO2 reduction. The membrane assisted in solubilizing higher amounts of CO2 and, as a result, significantly increased the reaction rate and changed the selectivity of the reaction due to the higher local concentration of the reactant in proximity to the electrocatalytic surface. We took advantage of this discovery to develop a better gas-diffusion electrode (GDE) that improves state-of-the-art performance.
In addition, we are working on ammonia electrosynthesis using heterogenized molecular catalysts in MOFs. We intend to elaborate more on the effect of proximal proton relays on catalytic rate and selectivity.
In addition, we are working on ammonia electrosynthesis using heterogenized molecular catalysts in MOFs. We intend to elaborate more on the effect of proximal proton relays on catalytic rate and selectivity.