Three-Dimensional-Structured Boron- and Nitrogen-Doped Graphene Hydrogel Enabling High-Sensitivity NO2 Detection at Room Temperature.

Abstract

Heteroatom-doping has been proved as an effective method to modulate the electronic, physical, and chemical properties of graphene (Gr). Developing a new strategy of heteroatom-doping for high-performance gas sensing is a pivotal issue. Here, we demonstrate novel Gr-based gas sensors through three-dimensional (3D)-structured B-/N-doping nanomaterials for high-performance NO2 sensing. The 3D porous B- and N-doped reduced graphene oxide hydrogels (RGOH) are synthesized via one-step hydrothermal self-assembly and employed as transducing materials to fabricate room-temperature high-performance chemiresistors. The systematic characterizations of the as-synthesized B- and N-RGOH clearly show the uniform doping of the B and N heteroatoms and the formation of B and N components with C/O. In comparison with the pristine RGOH counterpart, the 3D B- and N-RGOH sensors exhibit 38.9 and 18.0 times enhanced responses toward 800 ppb NO2, respectively, suggesting the remarkable doping effect of the heteroatoms in improving the sensitivity. Significantly, B- and N-RGOH display the exceptionally low limit of detection of 9 and 14 ppb NO2, respectively, which are much lower than the threshold limit recommended by the U.S. Environmental Protection Agency. In addition, the developed NO2 sensors show good linearity, reversibility, fast recovery, and impressive selectivity. This work opens up a new avenue to fabricate room-temperature and high-performance NO2 sensors by incorporating B and N heteroatoms into 3D RGOH via a convenient hydrothermal self-assembly approach.