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Atomically confined calcium in nitrogen-doped graphene as an efficient heterogeneous catalyst for hydrogen evolution.

ABSTRACT: Calcium is one of the most abundant and cheapest elements on earth. However, due to the lack of d-orbitals for chemical adsorption, it is generally considered as a stoichiometric reagent with no catalytic activities in heterogeneous catalysis. In this research, we have revealed that atomically confined Ca in nitrogen-doped graphene (Ca₁-NG) can be an effective heterogeneous catalyst to boost both electrocatalytic and photocatalytic hydrogen evolution reactions (HER). Ca single atoms anchored in NG can efficiently enhance the HER performance due to the improvement of the interfacial charge transfer rate and suppression of the photo-generated charge recombination. Density functional theory calculations show that the high catalytic activity of Ca₁-NG results from the Ca single atoms in NG, which leads to multiple H adsorption configurations with favorable ΔG_H∗ values for HER. This research can be valuable for the designing of environmentally friendly, economical and efficient catalysts for renewable hydrogen production.

SUBMITTER: Sun J

PROVIDER: S-EPMC8254045 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description:The development of a heterogeneous catalyst for use in environmental remediation remains a challenging and attractive research endeavor. Specifically, for Fenton reactions, most research approaches have focused on the preparation of iron-containing heterostructures as photo-Fenton catalysts that utilize visible light for enhancing the degradation efficiency. Herein, the synthesis and novel application of C,N-doped iron borates are demonstrated as single-component heterogeneous photo-Fenton catalysts with high Fenton activity under visible light. Under the optimal conditions, 10 mg of the catalyst is shown to achieve effective degradation of 10 ppm methylene blue (MB) dye, Rhodamine B (RhB) dye, and tetracycline (TC) under simulated solar irradiation with a first-order rate constant of k = 0.218 min-1, 0.177 min-1, and 0.116 min-1, respectively. Using MB as a model system, the C,N-doped iron borate exhibits 10- and 26-fold increases in catalytic activity relative to that of the 50 nm hematite nanoparticles and that of the non-doped iron borate, respectively, in the presence of H2O2 under the simulated solar irradiation. Furthermore, the optimum reaction conditions used only 320 equivalents of H2O2 with respect to the concentration of dye, rather than the several thousand equivalents of H2O2 used in conventional heterogeneous Fenton catalysts. In addition, the as-prepared C,N-doped iron borate achieves 75% MB degradation after 20 min in the dark, thus enabling the continuous degradation of pollutants at night and in areas with poor light exposure. The stability and recyclability of C,N-doped iron borate for the oxidation of MB was demonstrated over three cycles with insignificant loss in photo-Fenton activity. The high Fenton activity of the C,N-doped iron borate is considered to be due to the synergistic action between the negatively-charged borate ligands and the metal center in promoting the Fenton reaction. Moreover, carbon and nitrogen doping are shown to be critical in modifying the electronic structure and increasing the conductivity of the catalyst. In view of its synthetic simplicity, high efficiency, low cost of reagents, and minimal cost of operation (driven by natural sunlight), the as-prepared heterogeneous single-component metal borate catalyst has potential application in the industrial treatment of wastewater.

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Atomically confined calcium in nitrogen-doped graphene as an efficient heterogeneous catalyst for hydrogen evolution.

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