Towards stable solar water-splitting devices: elucidating the degradation kinetics in metal oxides-based photoelectrochemical devices

Lead Research Organisation: Imperial College London
Department Name: Chemistry

Abstract

Advanced economies, including European Union, have recently adopted or will soon announce hydrogen (H2) strategies targeting the broader goal of 'sector integration'. These strategies present a clear shift in global politics towards a net-zero approach in which H2 will play a major role to help decarbonize hard-to-electrify sectors. At present, however, industrial H2 is mainly produced by steam reforming of methane, which requires substantial hydrocarbon inputs and generates CO2 emissions. Photoelectrochemical (PEC) devices constitute one of the most challenging yet promising H2 production technologies, and can potentially achieve sustainable development of H2 energy in the future. However, until now, the investigation of environmentally friendly PEC systems for H2 production has been mainly focused on improving the solar-to-hydrogen (STH) efficiency while their stability and in particular the causes behind degradation, are less investigated. However, as scientists and engineers, it is important to develop new technologies in which the overall performances are taken into account, to pave the way for their commercial application. In RainDrop I tackle this issue, aiming to investigate the underlying causes of degradations of state-of-the-art metal oxides photoelectrodes and of their passivation layers, using a holistic approach that foresees the use of novel advanced methods based on in-situ and operando techniques. A wide range of spectroscopic and surface probe techniques will be used to develop a deeper understanding of the interplay between kinetics and energetics of the devices, and in particular how the dynamics and degradation processes are reciprocally influenced. Through iterative design the key factors of the degradation mechanisms will be identified and general materials design guidelines will be proposed to improve the stability of MOx-based PEC systems. Ultimately, an optimized MOx-PEC device will be assembled for obtaining a stable solar H2 generation.

Publications

10 25 50
 
Description Research ongoing.
Results to date have focused on photoactivation and photodegradation properties of Bismuth Vanadate photoelectrodes. This work is now being written up for publication and will be reported on in more detail in next years report
Exploitation Route The development of photoelectrodes and photocatalysts for Sunlight to fuels and chemicals with improved efficiency and stability
Sectors Energy

 
Description Solar Chemicals Network Travel Awards
Amount £700 (GBP)
Organisation Solar Fuels Network 
Sector Academic/University
Country United Kingdom
Start 11/2023 
End 02/2024
 
Description A spectroscopy investigation of Metal Oxide nanoparticles for water oxidation 
Organisation Dalian Institute of Chemical Physics
Country China 
Sector Private 
PI Contribution Our research team contributed by characterizing the samples using Photo-Induced Absorption (PIA) and Transient Absorption Spectroscopy (TAS). Specifically, we applied PIA spectroscopy to investigate the yield and kinetics of charge carriers in facet-engineered BiVO4 (F-BiVO4) and compared these findings with those of a non-faceted sample (NF-BiVO4) under various conditions. Our studies revealed that F-BiVO4 demonstrated superior charge separation behavior and an extended lifetime of charge carriers compared to NF-BiVO4, highlighting the effectiveness of facet engineering in enhancing photocatalytic performance.
Collaborator Contribution Prof. Can Li's group in Dalian successfully prepared PMMA-supported metal oxide nanoparticles, employing facet engineering techniques for some samples while leaving others unmodified. They have completed all preliminary morphological characterizations of these nanoparticles.
Impact This multidisciplinary collaboration, encompassing chemistry, engineering, photocatalysis, and physics, has significantly advanced the study of solar energy conversion using inorganic materials. Key outcomes include enhanced understanding of photocatalytic mechanisms and improved design of photocatalysts, demonstrating the synergy achieved by integrating expertise across different scientific disciplines.
Start Year 2023
 
Description Transient Absorption Spectroscopy study on ferromagnetic heterojunction 
Organisation Nankai University
Country China 
Sector Academic/University 
PI Contribution Our research team contributed to this collaboration by employing Transient Absorption Spectroscopy (TAS) to characterize the system and understand the impact of magnetic fields on charge separation and catalysis. This analysis is pivotal for enhancing the efficiency and understanding of the photoelectrochemical processes within the developed heterojunction thin films.
Collaborator Contribution Our partners, the Nankai and Alicante teams, have made contributions by preparing metal oxide/ferromagnetic heterojunction thin films for photoelectrochemical (PEC) cells. They have characterized these thin films, examining their morphology, magnetic effects, and performance, which are crucial aspects for enhancing the efficiency and understanding of PEC cells.
Impact This multidisciplinary collaboration, encompassing chemistry, engineering, photoelectrochemistry, and physics, has significantly advanced the study of solar energy conversion using inorganic materials. This collaboration has led to several key outcomes, including the development and characterization of innovative metal oxide/ferromagnetic heterojunction thin films for photoelectrochemical cells, and insights into the influence of magnetic fields on charge separation and catalysis
Start Year 2023
 
Description Transient Absorption Spectroscopy study on ferromagnetic heterojunction 
Organisation University of Alicante
Country Spain 
Sector Academic/University 
PI Contribution Our research team contributed to this collaboration by employing Transient Absorption Spectroscopy (TAS) to characterize the system and understand the impact of magnetic fields on charge separation and catalysis. This analysis is pivotal for enhancing the efficiency and understanding of the photoelectrochemical processes within the developed heterojunction thin films.
Collaborator Contribution Our partners, the Nankai and Alicante teams, have made contributions by preparing metal oxide/ferromagnetic heterojunction thin films for photoelectrochemical (PEC) cells. They have characterized these thin films, examining their morphology, magnetic effects, and performance, which are crucial aspects for enhancing the efficiency and understanding of PEC cells.
Impact This multidisciplinary collaboration, encompassing chemistry, engineering, photoelectrochemistry, and physics, has significantly advanced the study of solar energy conversion using inorganic materials. This collaboration has led to several key outcomes, including the development and characterization of innovative metal oxide/ferromagnetic heterojunction thin films for photoelectrochemical cells, and insights into the influence of magnetic fields on charge separation and catalysis
Start Year 2023
 
Description 1st UK Solar Chemicals Network Symposium 
Form Of Engagement Activity A talk or presentation
Part Of Official Scheme? No
Geographic Reach National
Primary Audience Postgraduate students
Results and Impact We contribute to Solar Chemicals Network (SCN) Symposium by presenting our latest research on "Photoactivation: Manipulating the Charge Dynamics of Metal Oxides Photoelectrodes with Light." Our work emphasizes the potential for photoactivation techniques to significantly improve the performance of solar energy devices by optimizing charge dynamics.
The symposium was attended by experts from various sectors, including PhD students, postdoctoral researchers, journal editors, and representatives from companies interested in the latest advancements in solar chemicals. This diverse audience facilitated a multidisciplinary dialogue, highlighting the current challenges and future directions in solar energy research. Our participation not only allowed us to showcase our findings but also to engage with other leading figures in the field, contributing to the ongoing efforts to develop sustainable solar energy solutions.
Year(s) Of Engagement Activity 2024
URL https://www.solarchemicals.co.uk/copy-of-1st-scn-symposium
 
Description CPE Solar [and Electro] Fuels Workshop 
Form Of Engagement Activity A talk or presentation
Part Of Official Scheme? No
Geographic Reach Local
Primary Audience Postgraduate students
Results and Impact At the CPE Solar and Electro Fuels Workshop, we had the opportunity to present our research focused on "Exploring the Impact of Interfaces and Environmental Factors on Water Oxidation Kinetics in Metal Oxides." The audience, primarily consisting of PhD students, showed great engagement with the topic. This presentation aimed to show several ways in which interfaces and environmental variables influence the efficiency and kinetics of water oxidation processes in metal oxides, a critical reaction for the production of solar fuels. The engagement of the audience highlighted the relevance and interest in understanding these complex interactions. This workshop served as a platform for sharing cutting-edge research and fostering discussions among emerging scientists about the challenges and opportunities in the development of more efficient solar fuels systems
Year(s) Of Engagement Activity 2023
URL https://www.imperial.ac.uk/events/167387/cpe-workshop-on-solar-fuels/
 
Description Future Energy Festival 2023 
Form Of Engagement Activity Participation in an activity, workshop or similar
Part Of Official Scheme? No
Geographic Reach Local
Primary Audience Public/other audiences
Results and Impact During this event, we contributed by "Shining a Light on Materials for Solar Energy Conversion." Our stand aimed to explain our research on green hydrogen to the general audience, explaining in layperson's terms how we utilize spectroscopy to investigate the process of water splitting. By breaking down complex scientific concepts into more understandable content, we sought to engage and educate the public on the importance of solar energy conversion and its potential to provide a sustainable source of green hydrogen.
Year(s) Of Engagement Activity 2023
URL https://www.imperial.ac.uk/events/164378/save-the-date-energy-futures-lab-future-energy-festival-202...
 
Description Global Hydrogen Production Technologies Center kickoff meeting 
Form Of Engagement Activity A formal working group, expert panel or dialogue
Part Of Official Scheme? No
Geographic Reach International
Primary Audience Other audiences
Results and Impact As part of the Global Hydrogen Production Technologies (HyPT) Center, an international partnership sponsored by the US, Australia, Canada, and the UK, we play a pivotal role in the development of inorganic photocatalyst materials for hydrogen production. This collaborative effort is distinguished as the first and currently unique National Science Foundation-funded hydrogen research initiative, encompassing seven countries, 20 universities, around 100 researchers, and an advisory board of 10 members from various sectors.
Our participation was highlighted through workshops and discussions focused on initiating our research collaborations with universities from the USA, Canada, Australia, and the UK. These sessions were instrumental in laying the groundwork for our project, facilitating the exchange of ideas, and setting strategic directions for leveraging the unique capabilities of each partner institution. The event not only showcased our commitment to advancing hydrogen technology through international collaboration but also underscored the importance of developing innovative photocatalyst materials. T
Year(s) Of Engagement Activity 2024
URL https://intheloop.engineering.asu.edu/2024/02/05/global-hydrogen-production-technologies-hypt-center...
 
Description Great Exhibition Road Festival 
Form Of Engagement Activity Participation in an activity, workshop or similar
Part Of Official Scheme? No
Geographic Reach Local
Primary Audience Public/other audiences
Results and Impact In collaboration with architecture firm Cookies, we showcased the benefits of developing durable cement through green methods that significantly reduce CO2 emissions. Throughout the day, a series of workshops were organized, engaging children aged 5 to 15 in the hands-on activity of molding various shapes using this "green cement." This interactive experience provided a practical understanding of the material's environmental advantages. The initiative aimed to foster awareness among the younger generation about sustainable building materials and their critical role in protecting the environment. The workshops sparked curiosity among participants about sustainable practices in construction.
Year(s) Of Engagement Activity 2023
URL https://www.greatexhibitionroadfestival.co.uk/event/down-earth/?backto=whats-on
 
Description Renewable Energy: Solar Fuels Gordon Research Conference 
Form Of Engagement Activity A talk or presentation
Part Of Official Scheme? No
Geographic Reach International
Primary Audience Postgraduate students
Results and Impact At the Renewable Energy: Solar Fuels Gordon Research Conference, we presented our research through a poster titled "A Spectroelectrochemical Study of Metal Oxides Photoelectrodes under Long-Term Illumination." Our study focused on the stability and efficiency of metal oxides in photoelectrocatalysis under prolonged illumination, addressing key challenges in the durability and performance of solar fuel generation components.
The presentation garnered significant interest from a diverse audience of PhD students, postdocs, industry professionals, and professors. These interactions provided valuable feedback and laid the groundwork for multiple collaborations, notably initiating partnerships between groups from Berkley National Lab, Yale, Boston University, and Imperial College London.
Year(s) Of Engagement Activity 2024
URL https://www.grc.org/renewable-energy-solar-fuels-conference/2024/