A NiRhS fuel cell catalyst – lessons from hydrogenase

Ogo, Seiji; Ando, Tatsuya; Minh, Le Tu Thi; Mori, Yuki; Matsumoto, Takahiro; Yatabe, Takeshi; Yoon, Ki Seok; Satô, Yukio; Hibino, Takashi; Kaneko, Kenji

doi:10.1039/d0cc04789a

Cited by 1 publication

(1 citation statement)

References 31 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…The establishment of a hydrogen-based economy remains a challenging task, and there is much one can learn from nature. Nowadays, there are several pathways to solve this problem by using different ways to produce and apply hydrogen, like making electrolytic devices [3], chemical fuel cells [4], artificial hydrogenases [5], and nanomaterials made of transition metal oxides [6]. The application of solar energy and hydrogenases is also a possible way, which is called photosynthesis.…”

Section: Introductionmentioning

confidence: 99%

Unveiling the Low-Lying Spin States of [Fe3S4] Clusters via the Extended Broken-Symmetry Method

Chu,

Gao

2024

Molecules

View full text Add to dashboard Cite

Photosynthetic water splitting, when synergized with hydrogen production catalyzed by hydrogenases, emerges as a promising avenue for clean and renewable energy. However, theoretical calculations have faced challenges in elucidating the low-lying spin states of iron–sulfur clusters, which are integral components of hydrogenases. To address this challenge, we employ the Extended Broken-Symmetry method for the computation of the cubane–[Fe3S4] cluster within the [FeNi] hydrogenase enzyme. This approach rectifies the error caused by spin contamination, allowing us to obtain the magnetic exchange coupling constant and the energy level of the low-lying state. We find that the Extended Broken-Symmetry method provides more accurate results for differences in bond length and the magnetic coupling constant. This accuracy assists in reconstructing the low-spin ground state force and determining the geometric structure of the ground state. By utilizing the Extended Broken-Symmetry method, we further highlight the significance of the geometric arrangement of metal centers in the cluster’s properties and gain deeper insights into the magnetic properties of transition metal iron–sulfur clusters at the reaction centers of hydrogenases. This research illuminates the untapped potential of hydrogenases and their promising role in the future of photosynthesis and sustainable energy production.

show abstract