Surface Engineering over Metal-Organic Framework Nanoarray to Realize Boosted and Sustained Urea Oxidation.

Facilitating C─N bond cleavage and promoting *COO desorption are essential yet challenging in urea oxidation reactions (UORs). Herein a novel interfacial coordination assembly protocol is established to modify the Co-phytate coordination complex on the Ni-based metal-organic framework (MOF) nanosheet array (CC/Ni-BDC@Co-PA) toward boosted and sustained UOR electrocatalysis. Comprehensive experimental and theoretical investigations unveil that surface Co-PA modification over Ni-BDC can manipulate the electronic state of Ni sites, and in situ evolved charge-redistributed surface can promote urea adsorption and the subsequent C─N bond cleavage.

3D Hierarchical-Architectured Nanoarray Electrode for Boosted and Sustained Urea Electro-Oxidation.

Exploring active and durable Ni-based materials with optimized electronic and architectural engineering to promote the urea oxidation reaction (UOR) is pivotal for the urea-related technologies. Herein a 3D self-supported hierarchical-architectured nanoarray electrode (CC/MnNi@NC) is proposed in which 1D N-doped carbon nanotubes (N-CNTs) with 0D MnNi nanoparticles (NPs) encapsulation are intertwined into 2D nanosheet aligned on the carbon cloth for prominently boosted and sustained UOR electrocatalysis. From combined experimental and theoretical investigations, Mn-alloying can regulate Ni electronic state with downshift of the d-band center, facilitating active Ni species generation and prompting the rate-determining step (*COO intermediate desorption).

Unconventional Phase Synergies with Doping Engineering Over Ni Electrocatalyst Featuring Regulated Electronic State for Accelerated Urea Oxidation.

Exploring high-performing Ni-based electrocatalysts for the urea oxidation reaction (UOR) is crucial for developing urea-related energy technologies yet remains a daunting challenge. In this study, a synergistic anomalous hcp phase and heteroatom doping engineering over metallic Ni are found to enhance the UOR. A metal-organic framework-mediated approach is proposed to construct Ni nanoparticles (NPs) with designated crystal phase embedded in N-doped carbon (fcc-Ni/NC and hcp-Ni/NC).

Encapsulated RuP-RuS nanoheterostructure with regulated interfacial charge redistribution for synergistically boosting hydrogen evolution electrocatalysis.

Exploring cost-effective electrocatalysts with suitable hydrogen binding strength and rational micro/nano-architecture towards the hydrogen evolution reaction (HER) is crucial for energy technologies, yet remains a tough challenge. Herein we present the first instance of a nanoscale RuP-RuS heterostructure encapsulated in N, P, and S co-doped porous carbon nanosheets (RuP-RuS/NPS-C) for boosting the HER. The synthesis involves the construction of a 2D core-shell structured precursor in which Ru-functionalized g-CN is wrapped by poly(cyclotriphosphazene--4,4'-sulfonyldiphenol) followed by pyrolysis.