Computational Design of Materials for Photocatalytic Hydrogen Generation and Separation

Project Information

Sol2H2

Grant agreement ID: 101031846

DOI

10.3030/101031846

Project closed

EC signature date 7 April 2021

Start date 15 September 2021

End date 14 September 2023

Funded under

• EXCELLENT SCIENCE - Marie Skłodowska-Curie Actions

Total cost

€ 162 806,40

EU contribution

€ 162 806,40

Coordinated by

HELMHOLTZ-ZENTRUM DRESDEN-ROSSENDORF EV
Germany

Periodic Reporting for period 1 - Sol2H2 (Computational Design of Materials for Photocatalytic Hydrogen Generation and Separation)

Reporting period: 2021-09-15 to 2023-09-14

Summary of the context and overall objectives of the project

The Sol2H2 project aims to tackle the critical challenge in the green energy generation and utilization based on the low-dimensional nanomaterials, including the efficient production and separation of hydrogen. Also, the optimization of water-associated reactions, specifically those integral to sustainable energy generation should also be addressed. Achieving efficient water-related reactions is essential for realizing the full potential of green and high-density energies such as hydrogen energy.

The Sol2H2 project is of important for society in three parts: 1) Transition to sustainable energy. This project contributes to the ongoing global transition to sustainable energy sources. By addressing challenges in hydrogen production or water-related reactions, the project plays a crucial role in facilitating a shift away from traditional, environmentally impactful energy sources. The green energy generation aligns with broader environmental sustainability goals. By promoting the efficient production of hydrogen, the project could help reduce reliance on fossil fuels, mitigating environmental impact, and addressing climate change concerns. 2) Unlocking the potential of hydrogen: Hydrogen is recognized as a clean and versatile energy carrier with the potential to significantly reduce greenhouse gas emissions. By overcoming challenges in hydrogen production and separation, the Sol2H2 project contributes to unlocking the full potential of hydrogen as a clean energy solution. 3) Responsible water resource management: optimizing water-associated reactions not only enhances energy generation processes but also aligns with responsible water resource management. As energy scarcity becomes a global concern, the project's emphasis on efficient water-related reactions contributes to the sustainable use of the numerous water resource.

In this project, we aim to demonstrate the hydrogen generation and separation process based on the low-dimensional based materials via ab initio calculations and dynamic simulations, to provide a knob for understanding the mechanism of proton tunneling, and further, the efficient water-related reaction and hydrogen generation for the wide practical application. Furthermore, we also expect to establish the relations between electronic structure and reaction performance, identify key electronic factors influencing reaction outcomes, and develop a rational design principle for materials with extraordinary performance in hydrogen-related reactions.

Work performed from the beginning of the project to the end of the period covered by the report and main results achieved so far

Over the past two years, our dedicated efforts have been focused on addressing the intricate challenges associated with hydrogen generation and separation, aiming to establish a rational design principle for materials exhibiting extraordinary performance in water/hydrogen-related processes.
1) Proton penetration mechanism and selective hydrogen isotope separation through two-dimensional biphenylene. Hydrogen isotope separation is of prime significance in various scientific and industrial applications. Nevertheless, the existing technologies are often expensive and energy demanding. Based on theoretical calculations, the proton penetration mechanism and the associated isotope separation behavior through two-dimensional biphenylene have been systematically investigated. We found that proton can readily pass through biphenylene with low energy barrier in some specific patterns. Furthermore, large kinetic isotope effect ratios for proton-deuteron (13.58) and proton-triton (53.10) were observed in aqueous environment. We thus conclude that biphenylene would be a potential carbon material used for hydrogen isotope separation. The insights garnered from this investigation are pivotal in advancing the exploration and identification of potential materials capable of serving as proton sieves. This has been made good progress in the projects with the publication of RSC Adv., 2023, 13, 27590.

2) Promoting oxygen reduction reaction on carbon-based materials by selective hydrogen bonding. Electrochemical oxygen reduction reaction (ORR) is fundamental for many energy conversion and storage devices. Using first-principles calculations, we elucidated how to rationally plant an additional *OH that can selectively interact with the ORR intermediate of *OOH via hydrogen bonding, while not affecting the *OH intermediate. This approach offers a great possibility for the rational design of efficient catalysts for ORR and other chemical reactions. This prompts a concerted effort toward the rational design of optimal catalysts for chemical reactions associated with energy processes. This work is in ChemSusChem2023,16, e2023000.

3) Utilizing high coordination diversity in carbon nanocone supported catalytic single-atom sites for screening of optimal activity. The hydrogen evolution reaction (HER) and oxygen reduction reaction (ORR) play pivotal roles in numerous energy conversion and storage technologies. However, engineering active sites to achieve optimal adsorption energy proves to be a challenging task. To address this, a novel design featuring transition metal single-atom active sites supported by carbon nanocone (CNC) with high coordination diversity is proposed through density functional theory calculations. The diverse electronic states of CNC carbon atoms impart varied coordination for the metal active sites, resulting in a nearly continuous distribution of adsorption energies for key intermediates. This research introduces a new strategy for crafting nanocone-based single-atom catalysts with promising catalytic performance, setting a novel guideline for the efficient design of the high-performance catalysts to advance the development of renewable energy technologies.

Progress beyond the state of the art and expected potential impact (including the socio-economic impact and the wider societal implications of the project so far)

In the Sol2H2 project, we've made groundbreaking progress in atomic-level structural design, enabling the creation of materials with exceptional performance in hydrogen generation/separation and water-associated reactions. This marks a significant leap forward in materials science for sustainable energy technologies.

We will continue to advance the related research efforts within this project. Some more outcomes could be expected: 1) Uncovering the causes and clarifying key factors in the proton tunneling process through the investigation of proton penetration on various candidates. 2) Providing further insights into the mechanisms governing hydrogen generation and separation 3) Continuing the refinement and optimization of atomic-level structural designs to maximize material performance in reactions. 4) Establishing robust correlations between material structure and performance.

The project's clarified mechanism and optimized materials can significantly impact socio-economic dynamics. Offering efficient solutions for hydrogen generation/separation and water-related reactions, these developments contribute to economic and social progress. The outcomes may have broader societal implications, advancing our understanding of fundamental energy conversion processes and informing future technologies aligned with sustainable energy goals. The project holds promise for technological advancements in novel materials, impacting industries like clean energy and materials science. The environmental impact lies in the rational design of materials, mitigating concerns and promoting cleaner, sustainable energy production in alignment with global ecological goals.