Sandwich-Structured Hybrid of NiCo Nanoparticles-Embedded Carbon Nanotubes Grafted on C₃N₄ Nanosheets for Efficient Photodehydrogenative Coupling Reactions

Abstract

Exploring cheap and efficient hybrid catalysts offers exciting opportunities for enhancing the performance of photocatalysts in the green organic synthesis field. Herein, a facile and effective approach is designed for the synthesis of a sandwich-structured hybrid in which NiCo bimetallic nanoparticles are embedded in the tip of nitrogen-doped carbon nanotubes (N-CNTs) grafted on both sides of a nitrogen deficient C3N4 (Nv-C3N4) nanosheet for photodehydrogenative coupling reactions. Such a brand-new type of sandwich-structured hybrid comprises Nv-C3N4 nanosheets and surrounding N-CNTs embedded with NiCo nanoparticles at their tips. Remarkably, the resultant hybrid exhibits integrated functionalities, abundant active sites, enhanced visible light absorption, and excellent interfacial charge transfer ability. As a result, the optimized NiCo@N-CNTs@Nv-C3N4 photocatalyst shows significantly improved photodehydrogenative coupling performance of amines to imines compared to the control single-metal-based catalysts (Ni@N-CNTs@Nv-C3N4 and Co@N-CNTs@Nv-C3N4). The mechanistic investigation through experimental and computational study demonstrates that, compared with single-metal-based hybrids, the NiCo bimetallic hybrid exhibits stronger amine adsorption and weaker photogenerated hydrogen atom adsorption, thus promoting the dehydrogenative activation of primary amines and fast generation of imines. This work presents a promising insight for designing and preparing efficient photocatalysts to trigger organic synthesis in high yields.

Cu-BTC-confined synthesis of Cu-Cu2O-CuS nanojunctions embedded in a porous carbon matrix for remarkable photothermal CO2conversion

“…S4†) presents two peaks at around 1340 and 1580 cm −1 , further revealing the existence of graphite in the hybrid. 36,37…”

“…S4 †) presents two peaks at around 1340 and 1580 cm −1 , further revealing the existence of graphite in the hybrid. 36,37 The elemental states of Cu-Cu 2 O-CuS@C were investigated by the XPS technique. In the survey XPS spectrum (Fig.…”

Nanomaterials in photocatalysed organic transformations: development, prospects and challenges

“…17). 165 g-C 3 N 4 and its doped analogues have been used for oxidation of the C-H bond, [166][167][168][169] amines, 145,[170][171][172] benzyl bromides, 173 benzyl [174][175][176] and other [177][178][179] alcohols, sulfinates, 180 and sulfides, 181 as well as for the oxidative amidation of aromatic aldehydes. 182,183 The oxidative coupling of aryl halides with tertiary amines could furnish various ketone derivatives in the presence of Ni/g-C 3 N 4 .…”

Electrochemiluminescence resonance energy transfer biosensing platform between g-C3N4 nanosheet and Ru–SiO2@FA for dual-wavelength ratiometric detection of SARS-CoV-2 RdRp gene

“…Graphitic carbon nitride nanosheets (g-C 3 N 4 NSs), as an emerging two-dimensional non-metallic semiconductor material, have been widely used and even sparked a gold rush in optoelectronics, catalysis and optical sensing fields for good electrical conductivity, well biocompatibility, and large specific surface area ( Ong et al, 2016 ; Volokh et al, 2019 ; Zhou et al, 2018 ). Furthermore, it was applied to construction of biosensors due to its excellent electrochemiluminescence properties ( Majdoub et al, 2020 ; Medetalibeyoğlu, 2021 ; Chen et al, 2022 ). Ru(bpy) 3 2+ as a classic ECL emitter displayed unparalleled ECL efficiency.…”