Photocatalytic N2 fixation has emerged as
one of the most useful ways to produce NH3, a useful asset
for chemical industries and a carbon-free energy source. Recently,
significant progress has been made toward designing efficient photocatalysts
to achieve this objective. Here, we introduce a highly active type-II
heterojunction fabricated via integrating two-dimensional (2D) nanosheets
of exfoliated g-C3N5 with nickel–chromium
layered double hydroxide (NiCr-LDH). With an optimized loading of
NiCr-LDH on exfoliated g-C3N5, excellent performance
is realized for green ammonia synthesis under ambient conditions without
any noble metal cocatalyst(s). Indeed, the g-C3N5/NiCr-LDH heterostructure with 2 wt % of NiCr-LDH (CN-NCL-2) exhibits
an ammonia yield of about 2.523 mmol/g/h, which is about 7.51 and
2.86 times higher than that of solo catalysts, i.e., NiCr-LDH (NC-L)
and exfoliated g-C3N5 (CN-5), respectively,
where methanol is used as a sacrificial agent. The enhancement of
NH3 evolution by the g-C3N5/NiCr-LDH
heterostructure can be attributed to the efficient charge transfer,
a key factor to the photocatalytic N2 fixation rate enhancement.
Additionally, N2 vacancies present in the system help adsorb
N2 on the surface, which improves the ammonia production
rate further. The best-performing heterostructure also shows long-term
stability with the NH3 production rate remaining nearly
constant over 20 h, demonstrating the excellent robustness of the
photocatalyst.