Formamidinium (FA)-rich lead iodide perovskite solar cells (PSCs) are gaining popularity because of their excellent photovoltaic performance. Nevertheless, the FA-rich perovskites processed by a two-step sequential deposition method usually possess...

HIGHLIGHTS • A novel N-doped strategy of C 2 N 3 − in situ trimerization between the 2D MXene interlayers was first proposed. • The ultra-fast pseudocapacitive behavior of Ti 3 C 2 T x /Na 3 TCM anode was managed and verified. • The as-fabricated sodium-ion capacitor delivers excellent electrochemical performance by anode/cathode mass matching. ABSTRACT 2D MXenes are attractive for energy storage applications because of their high electronic conductivity. However, it is still highly challenging for improving the sluggish sodium (Na)-ion transport kinetics within the MXenes interlayers. Herein, a novel nitrogen-doped Ti 3 C 2 T x MXene was synthesized by introducing the in situ polymeric sodium dicyanamide (Na-dca) to tune the complex terminations and then utilized as intercalation-type pseudocapacitive anode of Na-ion capacitors (NICs). The Na-dca can intercalate into the interlayers of Ti 3 C 2 T x nanosheets and simultaneously form sodium tricyanomelaminate (Na 3 TCM) by the catalyst-free trimerization. The as-prepared Ti 3 C 2 T x /Na 3 TCM exhibits a high N-doping of 5.6 at.% in the form of strong TiN bonding and stabilized triazine ring structure. Consequently, coupling Ti 3 C 2 T x /Na 3 TCM anode with different mass of activated carbon cathodes, the asymmetric MXene//carbon NICs are assembled. It is able to deliver high energy density (97.6 Wh kg −1), high power output (16.5 kW kg −1), and excellent cycling stability (≈ 82.6% capacitance retention after 8000 cycles).

A series of multiheteroatom porous carbon frameworks (MPCFs) is prepared successfully from the trimerization of cyano groups of our designed and synthesized 4,4'-(4-oxophthalazine-1,3(4H)-diyl)dibenzonitrile monomers and subsequent ionothermal synthesis. Benefiting from the molecular engineering strategy, the obtained MPCFs framework show a homogeneous distribution of nitrogen and oxygen heteroatoms at the atomic level, confirmed by the transmission electron microscopy mapping intuitively, thereby ensuring the stability of electrical properties. The supercapacitor with the obtained MPCFs@700 as the electrode exhibits a high energy density of 65 Wh kg at 0.1 A g, with excellent long cycle life and cycle stability (98% capacitance retention for 10 000 cycles in 1-butyl-3-methylimidazolium tetrafluoroborate). Another two electrolyte systems employed also demonstrate the delightful results, showing a 112% capacitance retention for 30 000 cycles in 1 M HSO and a 95% capacitance retention for 30 000 cycles in tetraethylammonium tetrafluoroborate in an acetonitrile solution. Moreover, the successful preparation of MPCFs provides new insights into the fabrication of electrode materials intrinsically containing nitrogen and oxygen in the frameworks for readily available components through a facile routine.