First-principles study of CO<sub>2</sub> hydrogenation to formic acid on single-atom catalysts supported on SiO<sub>2</sub>

Jun, Sun Hee; Jiang, Shuchao; Zhao, Yanliang; Wang, Honglei; Zhai, Dong; Deng, Weiqiao; Sun, Lei

doi:10.1039/d2cp02225g

Cited by 3 publications

(3 citation statements)

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“…A tremendously linear relationship of both the catalytic activity and the charge of the central metal was also found. 352 Similarly, Ni SA stabilized over O v defected Ti 3 C 2 O 2 (Ni@Ti 3 C 2 O 2 ) also favorable HCOOH generation and then quick desorption during the reaction process because of the smallest desorption barrier. 353 Furthermore, Cu SA-decorated C 2 N monolayer (Cu/C 2 N) for CO 2 hydrogenation to HCOOH was also investigated by DFT.…”

Section: Reviewmentioning

confidence: 99%

Recent advances of single-atom catalysts in CO₂ conversion

Wang

et al. 2023

Energy Environ. Sci.

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Section: Reviewmentioning

confidence: 99%

Recent advances of single-atom catalysts in CO₂ conversion

Wang

et al. 2023

Energy Environ. Sci.

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“…SAAs effectively merge the advantages of SACs and alloy structures, positioning them as potential candidates for CH 4 cracking catalysts 19 , 20 . The manipulation of SAAs’ performance can be achieved through the design of metal surface configurations and the variation of single-atom metal compositions, offering an avenue for catalyst development with high catalytic activity tailored to specific reactions 21 , 22 . However, the compositional space of SAAs is exceedingly extensive, and screening optimal compositions solely through experimental means proves to be time-consuming and labor-intensive.…”

Section: Introductionmentioning

confidence: 99%

Machine learning aided design of single-atom alloy catalysts for methane cracking

Sun,

Tu,

et al. 2024

Nat Commun

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The process of CH4 cracking into H2 and carbon has gained wide attention for hydrogen production. However, traditional catalysis methods suffer rapid deactivation due to severe carbon deposition. In this study, we discover that effective CH4 cracking can be achieved at 450 °C over a Re/Ni single-atom alloy via ball milling. To explore single-atom alloy catalysis, we construct a library of 10,950 transition metal single-atom alloy surfaces and screen candidates based on C–H dissociation energy barriers predicted by a machine learning model. Experimental validation identifies Ir/Ni and Re/Ni as top performers. Notably, the non-noble metal Re/Ni achieves a hydrogen yield of 10.7 gH2 gcat–1 h–1 with 99.9% selectivity and 7.75% CH4 conversion at 450 °C, 1 atm. Here, we show the mechanical energy boosts CH4 conversion clearly and sustained CH4 cracking over 240 h is achieved, significantly surpassing other approaches in the literature.

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“…In recent years, there has been an upsurge in modeling the phenomenon of hydrogen spillover theoretically using DFT . Many phenomena have been studied, including the correlation between charge transfer and structural properties, hydrogen adsorption energies, magnetic behavior, and electronic properties [55,81], formation energy, hydrogen dissociation capacity [57], H atom binding ability, and H 2 dissociation barriers [59], strategies for the reduction of H migration barrier in hydrogen spillover [62], preferred hydrogen adsorption sites [65], the role of the surface Brønsted acid sites (hydroxyl groups) in initiating H spillover [66], minimum-energy paths of H migration from a Pt catalyst to a WO 3 surface and bulk [81], to name but a few. However, DFT studies involving the calculation of vibrational densities of states relevant to the spillover process are very rare [60,79,80].…”

Section: Introductionmentioning

confidence: 99%

Hydrogen Spillover in Tungsten Oxide Bronzes as Observed by Broadband Neutron Spectroscopy

et al. 2023

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Hydrogen spillover is an elusive process, and its characterization, using experimental probes and ab initio modeling, poses a serious challenge. In this work, the nuclear quantum dynamics of hydrogen in a palladium-decorated cubic polymorph of tungsten oxide, Pd/cWO3, are characterized by the technique of neutron Compton scattering augmented by ab initio harmonic lattice modeling. The deeply penetrating nature of the neutron scattering process, the lack of spectroscopic selection rules, the inherent high sensitivity to hydrogen, the high energy and momentum resolution for hydrogen, and the mass selectivity of the technique render the neutron Compton scattering a very potent and unique tool for investigating the local dynamics of hydrogen species in bulk matrices. The total neutron Compton scattering response of hydrogen is described in terms of the hydrogen momentum distribution. The distribution is deconvoluted under the assumption of three pools of hydrogen with distinctly different nuclear quantum dynamical behavior: (i) hydrogen-terminated beta-palladium hydride, (ii) hydrogen in acid centers (OH+ groups) on the surface of the cubic phase of tungsten oxide, and (iii) quasi-free atomic hydrogen inside the saturated hydrogen bronze resulting from the spillover process. The ab initio modeling of lattice dynamics yields theoretical predictions for the values of the widths of proton momentum distributions in the first two hydrogen pools, which allows for obtaining the contribution and the width of the momentum distribution of the quasi-free atomic hydrogen resulting from the hydrogen spillover process. The analysis reveals that the local binding strength of the quasi-free hydrogen is characterized by the values of nuclear momentum distribution width, nuclear kinetic energy, and force constant of the underlying potential of the mean force close to those of free, unconstrained hydrogen atomic species in a gas of non-interacting particles described by the Maxwell–Boltzmann distribution. Moreover, this picture of the local dynamics of the quasi-free hydrogen is consistent with the proton polaron model of hydrogen-induced coloration of bulk hydrogenated WO3.

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First-principles study of CO₂ hydrogenation to formic acid on single-atom catalysts supported on SiO₂

Abstract: The hydrogenation of CO2 into valuable chemical fuels reduces the atmospheric CO2 content and also has broad economic prospects. Support is essential for catalysts, but many of the reported support...

Cited by 3 publications

References 61 publications

Recent advances of single-atom catalysts in CO₂ conversion

Recent advances of single-atom catalysts in CO₂ conversion

Machine learning aided design of single-atom alloy catalysts for methane cracking

Hydrogen Spillover in Tungsten Oxide Bronzes as Observed by Broadband Neutron Spectroscopy

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First-principles study of CO2 hydrogenation to formic acid on single-atom catalysts supported on SiO2

Abstract: The hydrogenation of CO2 into valuable chemical fuels reduces the atmospheric CO2 content and also has broad economic prospects. Support is essential for catalysts, but many of the reported support...

Cited by 3 publications

References 61 publications

Recent advances of single-atom catalysts in CO2 conversion

Recent advances of single-atom catalysts in CO2 conversion

Machine learning aided design of single-atom alloy catalysts for methane cracking

Hydrogen Spillover in Tungsten Oxide Bronzes as Observed by Broadband Neutron Spectroscopy

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First-principles study of CO₂ hydrogenation to formic acid on single-atom catalysts supported on SiO₂

Recent advances of single-atom catalysts in CO₂ conversion

Recent advances of single-atom catalysts in CO₂ conversion