A step‐by‐step strategy is reported for improving capacitance of supercapacitor electrodes by synthesizing nitrogen‐doped 2D Ti2CTx induced by polymeric carbon nitride (p‐C3N4), which simultaneously acts as a nitrogen source and intercalant. The NH2CN (cyanamide) can form p‐C3N4 on the surface of Ti2CTx nanosheets by a condensation reaction at 500–700 °C. The p‐C3N4 and Ti2CTx complexes are then heat‐treated to obtain nitrogen‐doped Ti2CTx nanosheets. The triazine‐based p‐C3N4 decomposes above 700 °C; thus, the nitrogen species can be surely doped into the internal carbon layer and/or defect site of Ti2CTx nanosheets at 900 °C. The extended interlayer distance and c‐lattice parameters (c‐LPs of 28.66 Å) of Ti2CTx prove that the p‐C3N4 grown between layers delaminate the nanosheets of Ti2CTx during the doping process. Moreover, 15.48% nitrogen doping in Ti2CTx improves the electrochemical performance and energy storage ability. Due to the synergetic effect of delaminated structures and heteroatom compositions, N‐doped Ti2CTx shows excellent characteristics as an electrochemical capacitor electrode, such as perfectly rectangular cyclic voltammetry results (CVs, R2 = 0.9999), high capacitance (327 F g−1 at 1 A g−1, increased by ≈140% over pristine‐Ti2CTx), and stable long cyclic performance (96.2% capacitance retention after 5000 cycles) at high current density (5 A g−1).

We report a strategy to turn non-electrocatalytic 2D-titanium carbide MXene (Ti2CTx) into a highly active electrocatalyst by nitridation with sodium amide (NaNH2).

Identifying effective means to improve the electrocatalytic performance of transition metal dichalcogenides in alkaline electrolytes is a significant challenge. Herein, an advanced electrocatalyst possessing shells of molybdenum disulfide (MoS2) on molybdenum carbide (Mo2C) for efficient electrocatalytic activity in alkaline electrolytes is reported. The strained sheets of curved MoS2 surround the surface of Mo2C, turning the inactive basal planes of MoS2 into highly active electrocatalytic sites in the alkaline electrolyte. The van der Waals layers, which even possess van der Waals epitaxy along (100) facets of MoS2 and Mo2C, enhance the spin coupling between MoS2 and Mo2C, providing an easy electron transfer path for excellent electrocatalytic activity in alkaline electrolytes and solving the stability issue. In addition, it is found that curved MoS2 sheets on Mo2C show 3.45% tensile strain in the lattice, producing excellent catalytic activity for both oxygen reduction reaction (ORR) (with E1/2 = 0.60 V vs RHE) and oxygen evolution reaction (OER) (overpotential = 1.51 V vs RHE at 10 mA cm−2) with 60 times higher electrochemical active area than pristine MoS2. The unique structure and synthesis route outlined here provide a novel and efficient approach toward designing highly active, durable, and cost‐effective ORR and OER electrocatalysts.

The ability to rapidly detect, identify, and monitor chemical warfare agents (CWAs) is imperative for both military and civilian defense. Since most CWAs and their simulants have an organophosphonate group, which is a hydrogen (H)-bond acceptor, many H-bond donors have been developed to effectively bind to the organophosphonate group. Although thioureas have been actively studied as an organocatalyst, they are relatively less investigated in CWA detection. In addition, there is a lack of studies on the structure-property relationship for gas phase detection. In this study, we synthesized various thioureas of different chemical structures, and tested them for sensing dimethylmethylphosphonate (DMMP), a CWA simulant. Molecular interaction between DMMP and thiourea was measured by H NMR titration and supported by density functional theory (DFT) calculations. Strong H-bond donor ability of thiourea may cause self-aggregation, and CH-π interaction can play an important role in the DMMP detection. Gas-phase adsorption of DMMP was also measured using a quartz crystal microbalance (QCM) and analyzed using the simple Langmuir isotherm, showing the importance of structure-induced morphology of thioureas on the surface.

Single-walled carbon nanotubes (SWCNTs) were fabricated using AC dielectrophoresis into chemocapacitive sensors, and molecular receptors were applied for the selective detection of several chemical warfare agents (CWAs). The selective responses toward nerve simulants (G and V), choking and blister agents as well as a pesticide were investigated with specific receptor molecules that were either covalently functionalized or noncovalently coated onto the surfaces of the SWCNTs. The SWCNT-based chemocapacitive sensors showed reproducibility and sensitivity to 200 ppb for several target molecules. The fabricated sensor arrays were assessed for the selective detection of six different CWAs, and the principal component analysis demonstrated their specificity. VX, a real nerve agent, was tested on the fabricated SWCNT-based chemocapacitive sensor coated with a thiourea-functionalized siloxane polymer, and the successful detection of VX at 100 ppb confirmed that our SWCNT-based sensors are suitable for practical applications.