large-scale application of this technology. Although Pt and Ru/Ir-based noble metal materials are the state-of-the-art electrocatalysts for overall water splitting, their applications are still limited by their scarcity and high price. Therefore, the design of low-cost and efficient electrocatalysts via eco-friendly synthesis strategies is highly desired and full of challenge. Among various nonprecious-metal-based electrocatalysts (such as transition metal chalcogenides, [2] nitrides, [3] and phosphides [4] ), transition metal phosphides (TMPs) have been widely investigated owing to their unique activities toward hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). The application of TMPs for HER is inspired by their outstanding properties as the active centers for hydro-desulfurization and hydrogenase-analogous catalytic mechanism in HER. Research results have demonstrated that the metal and phosphorous sites can transfer hydride and proton in the catalytic process, respectively, which contributes outstanding performance to TMPs for HER. [5] Besides the electrocatalytic properties toward HER, TMPs, especially Fe-, Co-, and Ni-based phosphides, also possess high activity to OER. [6] Experimental results have shown that the real catalytic sites are the TMP-derived surface oxides/ hydroxides and phosphates during electro-oxidation scan in the OER process. The phosphides are able to facilitate the in situ formation of active oxides/hydroxides and phosphates. [7] Thus efficient TMP electrocatalysts are highly desired in overall water splitting.Based on the advantages of carbon materials, compositing TMPs with nano-carbon matrix (TMPs@C) has been intensively designed to improve the electrocatalytic performance of single TMPs. [8] The introduced nano-carbon matrix can not only enhance the charge transfer but also facilitate the exposure of active sites. The introduction of nano-carbon into TMPs mainly involves two approaches: i) in situ converting metalorganic precursors through calcination; ii) directly compositing of pre-formed nano-carbons such as carbon nanotubes and graphene. Specifically, metal-organic framework (MOF)-derived strategy, belonging to the first approach, has recently emerged as an attractive route for constructing TMPs@C because of the uniform distribution of metal sites and organic ligands in MOFs. [9] The in situ carbonization of organic ligands around The development of low-cost and highly efficient electrocatalysts via an eco-friendly synthetic method is of great significance for future renewable energy storage and conversion systems. Herein, cobalt phosphides confined in porous P-doped carbon materials (Co-P@PC) are fabricated by calcinating the cobalt-phosphonate complex formed between 1-hydroxyethylidenediphosphonic acid and Co(NO 3 ) 2 in alkaline solution. The P-containing ligand in the complex acts as the carbon source as well as in situ phosphorizing agent for the formation of cobalt phosphides and doping P element into carbon material upon calcination. The Co-P@PC ...

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