H2S, a highly toxic chemical, is produced in massive quantities worldwide as a byproduct. Environmental regulations require >99% sulfur recovery, which is currently met using sulfur recovery units based on the Claus process, where H2S is converted to sulfur and water. Ideally, hydrogen in H2S is recovered as H2. Despite much effort to achieve this objective, especially in thermal catalysis, an industrial application remains distant. A fundamental factor is the lack of an effective catalyst. In this work, we employ density functional theory to illustrate the main limitations in existing catalysts. We use pure metals to explain this by studying the full elementary steps in H2S decomposition. We find that many catalysts, though capable of decomposing H2S, are limited due to sulfur poisoning. We conclude by outlining the ideal properties of a catalyst for this process.

Sulfur poisoning is a major challenge in catalytic processes where it can result in a gradual decline in the activity of the metal catalyst or a complete deactivation of the catalyst. Many studies were conducted to investigate the effects of sulfur poisoning on metals and address this challenge by developing a catalyst that is resistant to sulfur poisoning without compromising its performance. Boron doping showed to be a promising approach to modify the properties of metal catalysts and improve their performance in various applications. In this work, we conduct periodic density functional theory (DFT) calculations to study boron doping on a number of metals and its impact on sulfur poisoning. Our DFT calculations show that boron doping impacts metals differently. Boron doping is favourable on few metals (Pd, Pt, Rh and Ru) and very unfavourable on other metals (e.g. Ag and Cu). On Pd, Pt, and Rh, boron doping has a positive impact on reducing sulfur poisoning, with the impact varying with boron concentration. Finally, as a case study, we examine the impact of boron doping on H2S splitting to create H2 and show that boron doping has a pronounced positive impact on the performance of Pd-based catalyst.

H2S, a highly toxic chemical, is produced in massive quantities worldwide as a by-product. Environmental regulations require >99% sulfur recovery, which is currently met using sulfur recovery units based on the Claus process, where H2S is converted to sulfur and water. Ideally, hydrogen in H2S is recovered as H2. Despite much effort to achieve this objective, especially in thermal catalysis, an industrial application remains distant. A fundamental factor is the lack of an effective catalyst. In this work, we employ density functional theory (DFT) to illustrate the main limitations in existing catalysts. We use pure metals to explain this by studying the full elementary steps in H2S decomposition. We find that many catalysts, though capable of decomposing H2S, are limited due to sulfur poisoning. We conclude by outlining the ideal properties of a catalyst for this process.

Sulfur poisoning is a major challenge in catalytic processes where it can result in a gradual decline in the activity of the metal catalyst or a complete deactivation of the catalyst. Many studies were conducted to investigate the effects of sulfur poisoning on metals and address this challenge by developing a catalyst that is resistant to sulfur poisoning without compromising its performance. Boron doping showed to be a promising approach to modify the properties of metal catalysts and improve their performance in various applications. In this work, we conduct periodic density functional theory (DFT) calculations to study boron doping on a number of metals and its impact on sulfur poisoning. Our DFT calculations show that boron doping impacts metals differently. Boron doping is favourable on few metals (Pd, Pt, Rh and Ru) and very unfavourable on other metals (e.g. Ag and Cu). On Pd, Pt, and Rh, boron doping has a positive impact on reducing sulfur poisoning, with the impact varying with boron concentration. Finally, as a case study, we examine the impact of boron doping on H2S splitting to create H2 and show that boron doping has a pronounced positive impact on the performance of Pd-based catalyst.