The Sabatier principle defines the essential criteria
for being
an ideal catalyst in heterogeneous catalysis, while approaching the
Sabatier optimal is a major pursuit in catalyst design. The Haber–Bosch
(H-B) process, converting nitrogen (N2) and hydrogen (H2) to ammonia (NH3), is a holy grail reaction for
humans and also a great model reaction for fundamental research, where
the established volcano plot between ammonia synthesis activity and
nitrogen binding energy among metals has successfully guided new catalyst
design. However, reaching the top of the activity volcano is still
very challenging. Herein, we identify an elegant strategy to promote
the ferromagnetic (FM) catalysts to be the Sabatier optimal of ammonia
synthesis via a second-order ferromagnetic–paramagnetic phase
transition, which represents an ideal and novel interdisciplinary
of the aforementioned century-old classic principle, reaction, and
theory in chemistry, physics, and material science. The paramagnetic
(PM) Co and Ni metals could have 2–4 orders of magnitude higher
ammonia synthesis activity than their ferromagnetic counterparts,
holding the potential to achieve a near-ambient H-B process. We believe
that our discovery will open a novel avenue for revisiting the catalytic
performances of paramagnetic phases of ferromagnetic materials in
heterogeneous catalysis.
The catalytic carbon monoxide (CO) methanation is an ideal model reaction for the fundamental understanding of catalysis on the gas−solid interface and is crucial for various industrial processes. However, the harsh operating conditions make the reaction unsustainable, and the limitations set by the scaling relations between the dissociation energy barrier and dissociative binding energy of CO further increase the difficulty in designing high-performance methanation catalysts operating under milder conditions. Herein, we proposed a theoretical strategy to circumvent the limitations elegantly and achieve both facile CO dissociation and C/O hydrogenation on the catalyst containing a confined dual site. The DFT-based microkinetic modeling (MKM) reveals that the designed Co-Cr 2 /G dual-site catalyst could provide 4−6 orders of magnitude higher turnover frequency for CH 4 production than the cobalt step sites. We believe that the proposed strategy in the current work will provide essential guidance for designing state-of-the-art methanation catalysts under mild conditions.
Catalysis has played a crucial role in energy sustainability, environment control, and chemical production, while the design of high-performance catalysts is a key scientific question. In nature, biological organisms carry out catalysis with earth-abundant metals, whereas modern industrial processes rely heavily on precious metals. This points out the necessity of designing state-ofthe-art catalysts with earth-abundant elements to maintain sustainable catalysis. In this review, we will start with the fact that nature uses earth-abundant metals to feed the planet, followed by a few successful examples of catalyst design for water oxidation. Then, we will systematically introduce the practical methods in computational catalyst design and their applications in the rational modification of EAM catalysts for various reactions. In addition, the roles of high-throughput computations and artificial intelligence in this framework are summarized and discussed. We will also discuss the potential limitations of the framework and the strategies to overcome these challenges. Finally, we emphasize the importance of the synergistic efforts between theory and experiments in rational catalyst design with earth-abundant elements.
scite is a Brooklyn-based organization that helps researchers better discover and understand research articles through Smart Citations–citations that display the context of the citation and describe whether the article provides supporting or contrasting evidence. scite is used by students and researchers from around the world and is funded in part by the National Science Foundation and the National Institute on Drug Abuse of the National Institutes of Health.