Visible-light-driven organic transformations are of great interest in synthesizing valuable fine chemicals under mild conditions. The merger of heterogeneous photocatalysts and transition metal catalysts has recently drawn much attention due...

Metal phosphides have great potential for electrochemical energy-storage devices and electrocatalysis. Although monometallic and bimetallic phosphides have been extensively studied, the preparation of more complex metal phosphides remains challenging and it is necessary to further expand the available design space. Herein, we report a universal method to dope various metal cations into NiCoP nanocages (M-NiCoP, M = Al, Cu, Cr, Zn). Interestingly, the method can also be expanded to allow the incorporation of two to four metal dopants simultaneously (AlCu-NiCoP, AlZn-NiCoP, CrZn-NiCoP, AlCrCu-NiCoP, AlCrCuZn-NiCoP). To investigate the effect of incorporating multiple dopants, AlCu-NiCoP was used as the electrode material for supercapacitors, showing enhanced capacity and cycling stability compared to Al-NiCoP, Cu-NiCoP, and NiCoP electrodes. The superior electrochemical performance is attributed to the increased number of active sites, improved ion-diffusion kinetics, and a modulated electronic structure. An aqueous hybrid supercapacitor with AlCu-NiCoP as the positive electrode and activated carbon as the negative electrode was assembled and demonstrated a high energy density of 62.8 Wh kg–1 at a power density of 750 W kg–1 with good cycling stability.

Graphene-based magnetic materials exhibit novel properties and promising applications in the development of next-generation spintronic devices. Modern synthesis techniques have paved the way to design precisely the local environments of metal atoms anchored onto a nitrogen-doped graphene matrix. Herein, it is demonstrated that grafting cobalt (Co) into the graphene lattice induces robust and stable room-temperature ferromagnetism. These comprehensive experiments and first-principles calculations unambiguously identify that the mechanism for this unusual ferromagnetism is π-d orbital hybridization between Co d xz and graphene p z orbitals. Here, it is found that the magnetic interactions of Co-carbon ions are mediated by the spinpolarized graphene p z orbitals, and room temperature ferromagnetism can be stabilized by electron doping. It is also found that the electronic structure near the Fermi level, which sets the nature of spin polarization of graphene p z bands, strongly depends on the local environment of the Co moiety. This is the crucial, previously missing, ingredient that enables control of the magnetism. Overall, these observations unambiguously reveal that engineering the atomic structure of metal-embedded graphene lattices through careful d to p orbital interactions opens a new window of opportunities for developing graphene-based spintronics devices.

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