ERC FUNDED PROJECTS

The proposal is built on the core idea to use an ensemble of multiple level self-organization processes to create a next generation photocatalytic platform that provides unprecedented property and reactivity control. As a main output, the project will yield a novel highly precise combined catalyst/photocatalyst assembly to: 1) provide a massive step ahead in photocatalytic applications such as direct solar hydrogen generation, pollution degradation (incl. CO2 decomposition), N2 fixation, or photocatalytic organic synthesis. It will drastically enhance efficiency and selectivity of photocatalytic reactions, and enable a high number of organic synthetic reactions to be carried out economically (and ecologically) via combined catalytic/photocatalytic pathways. Even more, it will establish an entirely new generation of “100% depoisoning”, anti-aggregation catalysts with substantially enhanced catalyst life-time. For this, a series of self-assembly processes on the mesoscale will be used to create highly uniform arrays of single-catalyst-particle-in-a-single-TiO2-cavity; target is a 100% reliable placement of a single <10 nm particle in a 10 nm cavity. Thus catalytic features of, for example Pt nanoparticles, can ideally interact with the photocatalytic properties of a TiO2 cavity. The cavity will be optimized for optical and electronic properties by doping and band-gap engineering; the geometry will be tuned to the range of a few nm.. This nanoscopic design yields to a radical change in the controllability of length and time-scales (reactant, charge carrier and ionic transport in the substrate) in combined photocatalytic/catalytic reactions. It is of key importance that all nanoscale assembly principles used in this work are scalable and allow to create square meters of nanoscopically ordered catalyst surfaces. We target to demonstrate the feasibility of the implementation of the nanoscale principles in a prototype macroscopic reactor.

2 427 000 €

Start date: 2014-03-01, End date: 2019-02-28

The development of longer lasting, higher energy density and cheaper rechargeable batteries represents one of the major technological challenges of our society, batteries representing the limiting components in the shift from gasoline-powered to electric vehicles. They are also required to enable the use of more (typically intermittent) renewable energy, to balance demand with generation. This proposal seeks to develop and apply new NMR metrologies to determine the structure and dynamics of the multiple electrode-electrolyte interfaces and interphases that are present in these batteries, and how they evolve during battery cycling. New dynamic nuclear polarization (DNP) techniques will be exploited to extract structural information about the interface between the battery electrode and the passivating layers that grow on the electrode materials (the solid electrolyte interphase, SEI) and that are inherent to the stability of the batteries. The role of the SEI (and ceramic interfaces) in controlling lithium metal dendrite growth will be determined in liquid based and all solid state batteries. New DNP approaches will be developed that are compatible with the heterogeneous and reactive species that are present in conventional, all-solid state, Li-air and redox flow batteries. Method development will run in parallel with the use of DNP approaches to determine the structures of the various battery interfaces and interphases, testing the stability of conventional biradicals in these harsh oxidizing and reducing conditions, modifying the experimental approaches where appropriate. The final result will be a significantly improved understanding of the structures of these phases and how they evolve on cycling, coupled with strategies for designing improved SEI structures. The nature of the interface between a lithium metal dendrite and ceramic composite will be determined, providing much needed insight into how these (unwanted) dendrites grow in all solid state batteries. DNP approaches coupled with electron spin resonance will be use, where possible in situ, to determine the reaction mechanisms of organic molecules such as quinones in organic-based redox flow batteries in order to help prevent degradation of the electrochemically active species. This proposal involves NMR method development specifically designed to explore a variety of battery chemistries. Thus, this proposal is interdisciplinary, containing both a strong emphasis on materials characterization, electrochemistry and electronic structures of materials, interfaces and nanoparticles, and on analytical and physical chemistry. Some of the methodology will be applicable to other materials and systems including (for example) other electrochemical technologies such as fuel cells and solar fuels and the study of catalysts (to probe surface structure).

3 498 219 €

Start date: 2019-10-01, End date: 2024-09-30

Nanoparticles with etched substrate channels are proposed as a simplified enzyme mimic, nanozymes, for electrocatalysis providing concave catalytically active sites together with the local modulation of electrolyte composition. This concept will be extended to bimetallic core-shell structures with etched channels to provide locally confined catalyst surfaces with varying selectivity. The first catalytic reaction at the channel entrance selectively generates a product, which is further converted in a follow-up reaction catalysed at the core material at the bottom of the channel. The endeavour to locally assemble catalysts with different properties in nano-confined reaction volumes to actualise cascade reaction pathways will be extended to layered nanoparticle structures. Together with an anisotropic provision of a gaseous reactant through a hydrophobic/hydrophilic phase boundary of specifically designed gas diffusion electrodes multi-step catalytic cascade reactions become feasible. The development and extensive evaluation of multi-catalyst gas-diffusion electrodes using operando electrochemistry/spectroscopy and nano-electrochemical tools as well as multi flow-through electrolysers will provide the fundamental knowledge concerning the relative location of different catalyst particles, which synergistically perform chemical cascade reaction with high selectivity and at high current densities. These gas-diffusion electrodes will be integrated in novel electrolyser concepts targeting CO2 recycling at high current density in alkaline solution under suppression of H2 competition with previously unprecedented selectivity for the formation of higher hydrocarbons envisioning contributions to a closed carbon cycle economy and a substantial decrease of CO2 emission. Additionally, a novel tree-type rotating electrolyser design is proposed for the removal of hazardous gaseous pollutants from air e.g. at street crossings in cities as exemplified by NOx reduction to N2 or NH3.

2 499 462 €

Start date: 2019-09-01, End date: 2024-08-31

The widespread use of electronic devices, artificial light and rise of the 24-hour economy means that more individuals experience disruption of their chronotype, which is the natural circadian rhythm that regulates sleep and activity levels. The natural and medical sciences focus on the natural environment (e.g., light exposure), genetics, biology and health consequences, whereas the social sciences have largely explored the socio-environment (e.g., working regulations) and psychological and familial consequences of nonstandard work schedules. For the first time CHRONO bridges these disparate disciplines to ask: What is the role of biology, the natural and socio-environment and their interaction on predicting and understanding resilience to chronotype disruption and how does this in turn impact an individual’s health (sleep, cancer, obesity, digestive problems) and family (partnership, children) outcomes? I propose to: (1) develop a multifactor interdisciplinary theoretical model; (2) disrupt data collection by crowdsourcing a sociogenomic dataset with novel measures; (3) discover and validate with informed machine learning innovative measures of chronotype (molecular genetic, accelerometer, microbiome, patient-record, self-reported) and the natural and socio-environment; (4) ask fundamentally new substantive questions to determine how chronotype disruption influences health and family outcomes and, via Biology x Environment interaction (BxE), whether this is moderated by the natural or socio-environment; and, (5) develop new statistical models and methods to cope with contentious issues, answer longitudinal questions and engage in novel quasi-experiments (e.g., policy and life course changes) to transcend description to identify endogenous factors and causal mechanisms. Interdisciplinary in the truest sense, CHRONO will overturn long-held substantive findings of the causes and consequences of chronotype disruption.

2 499 811 €

Start date: 2019-11-01, End date: 2024-10-31