Journal
ADVANCED FUNCTIONAL MATERIALS
Volume 31, Issue 30, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adfm.202010912
Keywords
electrocatalytic overall water splitting; heteroatoms-doped carbon and graphene double-confinement; iron/nickel phosphides nanocrystals; nanohybrids; phase modulation
Categories
Funding
- National Natural Science Foundation of China [21671106, 11874334]
- National Key Research and Development Program of China [2019YFA 0307900]
- Priority Academic Program Development of Jiangsu Higher Education Institutions
- Opening Research Foundation from the State Key Laboratory of Coordination Chemistry, Nanjing National Laboratory of Solid State Microstructures, Nanjing University
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This study successfully synthesized phase-controlled iron/nickel phosphides nanocrystals coated with porous P-doped carbon and anchored on P-doped graphene, optimizing their surface/interface electronic structures and achieving the highest electrocatalytic activity for hydrogen and oxygen evolution in alkaline media. These pure-phase phosphides nanohybrids showed exceptional performance as bifunctional catalysts for water splitting, surpassing mixed phase and monometallic counterparts and previously reported catalysts based on Pt/C or IrO2.
Transition metal phosphides (TMPs) nanostructures have emerged as important electroactive materials for energy storage and conversion. Nonetheless, the phase modulation of iron/nickel phosphides nanocrystals or related nanohybrids remains challenging, and their electrocatalytic overall water splitting (OWS) performances are not fully investigated. Here, the phase-controlled synthesis of iron/nickel phosphides nanocrystals armored with porous P-doped carbon (PC) and anchored on P-doped graphene (PG) nanohybrids, including FeP-Fe2P@PC/PG, FeP-(NixFe1-x)(2)P@PC/PG, (NixFe1-x)(2)P@PC/PG, and Ni2P@PC/PG, are realized by thermal conversion of predesigned supramolecular gels under Ar/H-2 atmosphere and tuning Fe/Ni ratio in gel precursors. Thanks to phase-modulation-induced increase of available catalytic active sites and optimization of surface/interface electronic structures, the resultant pure-phase (NixFe1-x)(2)P@PC/PG exhibits the highest electrocatalytic activity for both hydrogen and oxygen evolution in alkaline media. Remarkably, using it as a bifunctional catalyst, the fabricated (NixFe1-x)(2)P@PC/PG parallel to(NixFe1-x)(2)P@PC/PG electrolyzer needs exceptional low cell voltage (1.45 V) to reach 10 mA cm(-2) water-splitting current, outperforming its mixed phase and monometallic phosphides counterparts and recently reported bifunctional catalysts based devices, and Pt/C parallel to IrO2 electrolyzer. Also, such (NixFe1-x)(2)P@PC/PG parallel to(NixFe1-x)(2)P@PC/PG device manifests outstanding durability for OWS. This work may shed light on optimizing TMPs nanostructures by combining phase-modulation and heteroatoms-doped carbon double-confinement strategies, and accelerate their applications in OWS or other renewable energy options.
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