Graphitic carbon nitrides as platforms for single-atom photocatalysis

Abstract

Herein we demonstrate that adding single-atoms of selected transition metals to graphitic carbon nitrides allow the tailoring of their electronic and chemical properties of these 2D nanomaterials, directly impacting their...

Metal-Free Photocatalysis: Two-Dimensional Nanomaterial Connection toward Advanced Organic Synthesis

“… 47 − 51 Moreover, PHI-CN materials offer another interesting opportunity in that the alkaline metals could be replaced by other transition metals through cation exchange strategies, thus potentially leading to CN–single atom materials. 52 …”

Themis: A Software to Assess Association Free Energies via Direct Estimative of Partition Functions

“…This enables the comparison of forcefields with higher theory methods such as DFT, which are too costly to be applied even for small clusters. It was also possible to study the interaction of carbon nitride sheets in order to build a multilayer structure and its further interaction with different cations 27 to build a single-cation catalyst using quantum chemistry energies from the GFN1-xTB Hamiltonian. 28 These very successful applications of our method within a quantum chemical potential energy surface might seem enough to prove the effectiveness of our proposal, but we will now present the proof of concept for a more complex application which raises a considerable interest in applied problems ranging from chemistry to biology and materials science: the thermodynamics of interactions involving electronic excited states.…”

Single-atom catalysts for high-efficiency photocatalytic and photoelectrochemical water splitting: distinctive roles, unique fabrication methods and specific design strategies

“…The ion exchange strategy was reported to be another facile wet-chemistry route to fabricate SACs. 126,180,181 Zeng et al demonstrated that Pt SAs with a high loading amount of 8.7 wt% were conned in the interlayer nanospace of g-C 3 N 4 by the ion exchange method (Fig. 6a), showing an enhanced photocatalytic HER performance due to the reduced proton transfer barrier induced by charge polarization effects around Pt SAs.…”

“…Colombari et al have employed poly(heptazine imides) (PHIs) as 2D substrates to successfully fabricate various SAbased photocatalysts (e.g., Ni, Pt and Ru) by the ion exchange method without introducing other metal ions as exchange sites in the fabrication of SACs based on g-C 3 N 4 -K 126 due to the more coordination possibilities of the heptazine rings in PHIs to anchor metal SAs. 180 In such an ion exchange method, the substrate powders were simply dispersed in the metal solutions (RuCl 3 , NiCl 2 or H 2 PtCl 6 ) to atomically anchor metal species. In another study, Yu et al have employed calcium alginate hydrogel (AG-Ca) as a starting substrate for the loading of Cu SAs by the ion exchange route for the electrocatalytic oxygen reduction reaction (ORR).…”

“…181 The Ca + ions in AG-Ca hydrogel were replaced by H + to obtain AG-H intermediates, which were then used to exchange copper ions in the solution to form metal-anchored carbon precursors. However, the intermediate state was not required in the fabrication of the aforementioned g-C 3 N 4 and PHI substrates for ion exchange procedures, 126,180 implying that the ions in the ion exchange route should be rationally selected in SAC fabrication for various catalytic reactions.…”