Periodic Reporting for period 4 - KIDS (Kinetics and Dynamics at Surfaces)
Reporting period: 2024-03-01 to 2025-08-31
Chemical reactions at solid surfaces lie at the heart of many processes that sustain modern society. From the production of clean fuels and fertilizers to the control of air pollutants and the conversion of energy in devices, heterogeneous catalysis is a cornerstone of industrial chemistry. Yet, despite its central role, our microscopic understanding of how individual molecules react on metal surfaces—how they bind, diffuse, transform, and release products—remains incomplete. This knowledge gap limits the rational design of new catalysts that are more efficient, selective, and environmentally friendly.
The project set out to address this challenge by developing and applying advanced experimental methods to observe catalytic reactions at surfaces with unprecedented resolution. Using molecular beams, ion imaging, and newly developed velocity-resolved kinetics techniques, we were able to measure reaction rates and identify transient intermediates at the atomic scale, under conditions approaching those in real catalytic systems. These approaches made it possible to disentangle complex reaction networks and quantify fundamental processes such as adsorption, diffusion, bond breaking, and tunneling at high temperatures.
Over the course of the project, significant milestones were achieved. We developed high-speed, multi-mass ion imaging detectors capable of acquiring data at rates up to 100 kHz, enabling simultaneous tracking of multiple reaction products. We identified key intermediates in the decomposition of formic acid on palladium, clarified the mechanism and rate-determining step of catalytic ammonia oxidation, and provided the first experimental evidence for cooperative adsorbate binding in hydrogen oxidation at elevated temperatures. Our work also demonstrated quantum tunneling effects in thermal reaction rates on metal surfaces and revealed how electronic non-adiabaticity modifies scattering and adsorption dynamics. These insights were published in leading journals including Science, Nature Reviews Chemistry, Journal of the American Chemical Society, ACS Catalysis, and Faraday Discussions.
The conclusions of the project are clear: by combining state-of-the-art instrumentation with rigorous theoretical collaboration, it is possible to establish quantitative benchmarks for catalytic surface chemistry that were previously inaccessible. These benchmarks not only resolve long-standing puzzles—such as the unexpectedly fast oxidation of hydrogen on platinum—but also provide guiding principles for catalyst design at the molecular level.
For society, the impact is twofold. First, the fundamental knowledge gained advances our ability to design catalysts that use less energy and produce fewer unwanted by-products, directly supporting cleaner industrial processes and more sustainable energy conversion. Second, the development of new experimental tools and methods ensures that the scientific community has the capability to probe increasingly complex catalytic systems, laying the groundwork for future innovation. In short, the project has delivered on its objectives: to deepen our fundamental understanding of surface-catalyzed chemistry and to equip researchers with new tools to meet the pressing energy and environmental challenges of our time.
The project set out to address this challenge by developing and applying advanced experimental methods to observe catalytic reactions at surfaces with unprecedented resolution. Using molecular beams, ion imaging, and newly developed velocity-resolved kinetics techniques, we were able to measure reaction rates and identify transient intermediates at the atomic scale, under conditions approaching those in real catalytic systems. These approaches made it possible to disentangle complex reaction networks and quantify fundamental processes such as adsorption, diffusion, bond breaking, and tunneling at high temperatures.
Over the course of the project, significant milestones were achieved. We developed high-speed, multi-mass ion imaging detectors capable of acquiring data at rates up to 100 kHz, enabling simultaneous tracking of multiple reaction products. We identified key intermediates in the decomposition of formic acid on palladium, clarified the mechanism and rate-determining step of catalytic ammonia oxidation, and provided the first experimental evidence for cooperative adsorbate binding in hydrogen oxidation at elevated temperatures. Our work also demonstrated quantum tunneling effects in thermal reaction rates on metal surfaces and revealed how electronic non-adiabaticity modifies scattering and adsorption dynamics. These insights were published in leading journals including Science, Nature Reviews Chemistry, Journal of the American Chemical Society, ACS Catalysis, and Faraday Discussions.
The conclusions of the project are clear: by combining state-of-the-art instrumentation with rigorous theoretical collaboration, it is possible to establish quantitative benchmarks for catalytic surface chemistry that were previously inaccessible. These benchmarks not only resolve long-standing puzzles—such as the unexpectedly fast oxidation of hydrogen on platinum—but also provide guiding principles for catalyst design at the molecular level.
For society, the impact is twofold. First, the fundamental knowledge gained advances our ability to design catalysts that use less energy and produce fewer unwanted by-products, directly supporting cleaner industrial processes and more sustainable energy conversion. Second, the development of new experimental tools and methods ensures that the scientific community has the capability to probe increasingly complex catalytic systems, laying the groundwork for future innovation. In short, the project has delivered on its objectives: to deepen our fundamental understanding of surface-catalyzed chemistry and to equip researchers with new tools to meet the pressing energy and environmental challenges of our time.
From the outset, the project focused on developing new experimental tools to observe catalytic reactions at surfaces with high sensitivity and time resolution, and then applying these tools to answer long-standing questions in heterogeneous catalysis.
Development of new instrumentation
A major achievement was the design of ion-imaging detectors capable of operating at extremely high count rates. These advances allowed data collection at up to 100 kHz, making it possible to follow multiple products simultaneously with both mass and velocity resolution. Such developments, reported in Review of Scientific Instruments (2025), represent a step-change in surface reaction kinetics experiments, opening the door to measurements that were previously impossible.
Fundamental insights into catalytic mechanisms
With these tools, we investigated several important catalytic processes:
• Hydrogen oxidation and ammonia conversion: We demonstrated that cooperative adsorbate binding catalyzes hydrogen oxidation on palladium at high temperatures (Science, 2024), and identified the mechanism and rate-determining step of ammonia oxidation on stepped palladium surfaces (ACS Catalysis, 2025). These studies resolve long-standing puzzles about how these critical industrial reactions proceed.
• Quantum effects in surface chemistry: We provided direct experimental evidence of tunneling in thermal reaction rates (Science, 2022), highlighting how quantum mechanics influences surface catalysis even at high temperatures.
• Formic acid decomposition and CO2 functionalization: By identifying transient intermediates and measuring adsorption and binding energies (Faraday Discussions, 2024; J. Phys. Chem. A, 2023; J. Phys. Chem. A, 2021), we mapped in detail how small organic molecules interact with metal surfaces — insights relevant to both sustainable fuels and CO2 utilization.
• Ammonia desorption and diffusion: We quantified how oxygen co-adsorption modifies ammonia mobility on platinum, affecting the efficiency of the Ostwald process (JACS, 2021, 2022).
General theoretical benchmarks
Through combined experiment and theory, we established quantitative benchmarks for surface kinetics. Our Nature Reviews Chemistry article (2019) synthesized the progress and challenges in the field, providing the community with a framework for interpreting reaction dynamics at surfaces.
Exploitation and dissemination
The results were widely disseminated through high-profile publications in Science, Nature Reviews Chemistry, JACS, ACS Catalysis, and other leading journals, as well as invited conference presentations and workshops. Beyond the scientific community, the new insights inform catalyst design strategies with potential applications in cleaner industrial processes, more efficient energy conversion, and the development of sustainable chemical pathways. The instrumentation itself has broad applicability and is already being adopted by other laboratories, ensuring long-term exploitation of the project’s achievements.
Overall conclusion
The project successfully delivered on its objectives: advancing the experimental methodology for probing catalytic reactions at surfaces, resolving critical mechanistic questions in hydrogen, ammonia, and formic acid chemistry, and providing a body of knowledge and tools that will be exploited both scientifically and industrially in the years ahead.
Development of new instrumentation
A major achievement was the design of ion-imaging detectors capable of operating at extremely high count rates. These advances allowed data collection at up to 100 kHz, making it possible to follow multiple products simultaneously with both mass and velocity resolution. Such developments, reported in Review of Scientific Instruments (2025), represent a step-change in surface reaction kinetics experiments, opening the door to measurements that were previously impossible.
Fundamental insights into catalytic mechanisms
With these tools, we investigated several important catalytic processes:
• Hydrogen oxidation and ammonia conversion: We demonstrated that cooperative adsorbate binding catalyzes hydrogen oxidation on palladium at high temperatures (Science, 2024), and identified the mechanism and rate-determining step of ammonia oxidation on stepped palladium surfaces (ACS Catalysis, 2025). These studies resolve long-standing puzzles about how these critical industrial reactions proceed.
• Quantum effects in surface chemistry: We provided direct experimental evidence of tunneling in thermal reaction rates (Science, 2022), highlighting how quantum mechanics influences surface catalysis even at high temperatures.
• Formic acid decomposition and CO2 functionalization: By identifying transient intermediates and measuring adsorption and binding energies (Faraday Discussions, 2024; J. Phys. Chem. A, 2023; J. Phys. Chem. A, 2021), we mapped in detail how small organic molecules interact with metal surfaces — insights relevant to both sustainable fuels and CO2 utilization.
• Ammonia desorption and diffusion: We quantified how oxygen co-adsorption modifies ammonia mobility on platinum, affecting the efficiency of the Ostwald process (JACS, 2021, 2022).
General theoretical benchmarks
Through combined experiment and theory, we established quantitative benchmarks for surface kinetics. Our Nature Reviews Chemistry article (2019) synthesized the progress and challenges in the field, providing the community with a framework for interpreting reaction dynamics at surfaces.
Exploitation and dissemination
The results were widely disseminated through high-profile publications in Science, Nature Reviews Chemistry, JACS, ACS Catalysis, and other leading journals, as well as invited conference presentations and workshops. Beyond the scientific community, the new insights inform catalyst design strategies with potential applications in cleaner industrial processes, more efficient energy conversion, and the development of sustainable chemical pathways. The instrumentation itself has broad applicability and is already being adopted by other laboratories, ensuring long-term exploitation of the project’s achievements.
Overall conclusion
The project successfully delivered on its objectives: advancing the experimental methodology for probing catalytic reactions at surfaces, resolving critical mechanistic questions in hydrogen, ammonia, and formic acid chemistry, and providing a body of knowledge and tools that will be exploited both scientifically and industrially in the years ahead.
The project has delivered a significant breakthrough in experimental methodology for studying surface reaction dynamics. We developed a technique capable of extracting complete kinetic traces with a temporal resolution of just 10 microseconds, captured with every single pulse of reactant. This represents a decisive step beyond the state of the art: whereas previous methods provided only partial or time-averaged information, our approach offers real-time access to the full evolution of a reaction.
A key advantage of this innovation is its ability to simultaneously deliver both total product yields and detailed kinetic data across a range of reactant concentrations. In practical terms, researchers can now obtain an entire kinetic profile from a single experiment, rather than piecing together individual data points over long acquisition times. This efficiency gain is dramatic—data acquisition rates are improved by roughly a factor of 1000 compared to conventional methods.
By the end of the project, we expect this methodology to become a routine tool for benchmarking catalytic systems and to be adopted by other laboratories worldwide. Its application will enable breakthroughs in understanding the mechanisms of industrially and environmentally important reactions, from clean energy conversion to sustainable chemical processes. In doing so, the project establishes a new experimental standard for heterogeneous catalysis with wide-ranging implications for catalyst design, energy efficiency, and environmental sustainability.
A key advantage of this innovation is its ability to simultaneously deliver both total product yields and detailed kinetic data across a range of reactant concentrations. In practical terms, researchers can now obtain an entire kinetic profile from a single experiment, rather than piecing together individual data points over long acquisition times. This efficiency gain is dramatic—data acquisition rates are improved by roughly a factor of 1000 compared to conventional methods.
By the end of the project, we expect this methodology to become a routine tool for benchmarking catalytic systems and to be adopted by other laboratories worldwide. Its application will enable breakthroughs in understanding the mechanisms of industrially and environmentally important reactions, from clean energy conversion to sustainable chemical processes. In doing so, the project establishes a new experimental standard for heterogeneous catalysis with wide-ranging implications for catalyst design, energy efficiency, and environmental sustainability.