Developing efficient and nonprecious large-current-density based oxygen evolution reaction (OER) electrocatalysts is strongly required for sustainable industrial water splitting. Hence, a unique heterostructure erecting by Mo-doped CoFe layered double hydroxides coating NiCo 2 S 4 nanotube arrays grown on nickel foam (NCS@CFM-LDH/NF) is elaborately demonstrated. It only needs an overpotential of 295/332 mV to achieve current density of 500/1000 mA cm -2 , respectively, with a low Tafel slope of 83.0 mV dec -1 in alkaline media. NCS@CFM-LDH/NF also shows an ultra-long-term stability at 1000 mA cm -2 over 100 h. Its remarkable performance is ascribed to the synergic effect of multi-component and hierarchical structure. Additionally, Theoretical calculations disclose that the doping of molybdenum is beneficial to the adsorption of the *O intermediate, thus promotes OER activity. This study provides an attractive approach to design highly active and durable OER catalysts for industrial application in electrolysis of water. • The unique nanotube arrays NCS@CFM 0.075 -LDH/NF catalyst has been prepared. • NCS@CFM 0.075 -LDH/NF presents good catalytic performance in alkaline media. • The dual electronic regulation effect greatly enhances the OER activity. • The 3D heterostructure provides superhydrophilic and superaerophobic surfaces. • DFT calculations show that the doping of Mo changes the RDS of the OER reaction. 

Construction Dual-regulated NiCo2S4@Mo-doped CoFe-LDH for Oxygen Evolution Reaction at Large Current Density

Cation modulation engineering is employed to tune the intrinsic activity and electronic structure of electrocatalysts for water electrolysis. Here, we designed two-dimensional cobalt–iron-layered double-hydroxide (CoFe-LDH) ultrathin nanosheets by pulsed laser ablation in an aqueous medium. The CoFe-LDH nanosheets exhibited abundant electrochemically active sites and a large surface area. The optimal Co0.5Fe0.5-LDH exhibited a low overpotential of 270 mV during half-cell oxygen evolution reactions (OERs), whereas Co0.25Fe0.75-LDH delivered 365 mV at 10 mA/cm2 during hydrogen evolution reactions (HERs). The bifunctional electrocatalyst exhibited an outstanding water electrolyzer performance at a cell voltage of ∼1.89 V at 10 mA/cm2 and admirable stability for long-run repetitive cycles. The synergistic effect between the modulated cations resulted in better conductivity, and the mass transfer facilitated the HER and OER. We demonstrated that this facile approach can facilitate the engineering of a highly stable and efficient electrode for renewable electrochemical energy conversion reactions. 

Dual-Cation-Coordinated CoFe-Layered Double-Hydroxide Nanosheets Using the Pulsed Laser Ablation Technique for Efficient Electrochemical Water Splitting: Mechanistic Screening by In Situ/Operando Raman and Density Functional Theory Calculations

Excessive emissions of cow manure have put tremendous pressure on environment, the difficulties in disposal methods have presented serious challenges to the livestock industry. Herein, cow manure biochar (CMB) loaded metal-organic framework (ZIF-67) precursors derived Co nanoparticles carbon (Co@NPC) at different temperatures to form biochar-based composites, i.e. , Co@NPC-CMB-x. The novel non-homogeneous catalysts activated peroxymonosulfate (PMS) to degrade the carbamazepine (CBZ). The results demonstrated that the pyrolysis temperature directly influenced the intrinsic properties and catalytic ability of products, with the higher pyrolysis temperature favoring the conversion of more graphitic C and graphitic N as active sites. In particular, Co@NPC-CMB-800 showed excellent activation of PMS, degrading 100% CBZ within 30 min. The high specific surface area, highly graphitic structure and the uniform dispersion of cobalt species were the key reasons for the excellent catalytic ability. X-ray photoelectron spectroscopy (XPS) illustrated that the interaction between biochar and transition metal was responsible to generate more reactive oxygen species. Furthermore, electron paramagnetic resonance (EPR) confirmed that non-radical singlet oxygen is the dominant pathway for CBZ degradation by the catalyst. This study provides a new strategy for cow manure application in functional catalysts and offers new prospects for designing efficient biochar-based catalysts for environmental remediation. The degradation mechanisms of CBZ in Co@NPC-CMB/PMS system • Biochar exhibits excellent catalytic performance of Co 2+ /PMS system. • The synergistic effect of Co/CMB effective enhance the redox cycle. • Non-radical pathway is the dominant pathway for CBZ degradation • The reaction mechanism of CBZ degradation by Co@NPC-CMB/PMS system is proposed. 

Co-ZIF reinforced cow manure biochar (CMB) as an effective peroxymonosulfate activator for degradation of carbamazepine

MXenes have been extensively studied due to their high metallic conductivity, hydrophilic properties, tunable layer structure and attractive surface chemistry, making them highly desirable for energy-related applications. However, slow catalytic reaction kinetics and limited active sites have severely impeded their further practical applications. Surface engineering of MXenes has been rationally designed and investigated to regulate their electronic structure, increase the density of active sites, optimize the binding energy, and thus boost the electrocatalytic performance. In this review, we comprehensively summarized the surface engineering strategies for MXene nanostructures, including surface termination engineering, defect engineering, heteroatom doping engineering (metals or non-metals), secondary material engineering, and extension to MXene analogues. By identifying the roles of each component in the engineered MXenes at the atomic level, their intrinsic active sites have been discussed to establish the relationships between the atomic structures and catalytic activities. We highlighted the state-of-the-art progress of MXenes in electrochemical conversion reactions including hydrogen, oxygen, carbon dioxide, nitrogen and sulfur conversion reactions. The challenges and perspectives of MXene-based catalysts for electrochemical conversion reactions are presented to inspire more efforts toward the understanding and development of MXene-based materials to meet the ever-growing demand for a sustainable future.

Engineering strategies and active site identification of MXene-based catalysts for electrochemical conversion reactions.

Recent Developments of MXene-based Catalysts for Hydrogen Production by Water Splitting

Metal-organic framework (MOF)-based materials are regarded as potential electrocatalysts for oxygen evolution reaction (OER) resulting from the abundant pore structures, large surface area and atomically dispersed metal centers, while their coordinately saturated metal nodes are inert to electrocatalysis. In this work, creating active sites while accelerating charge transport is proposed to improve the OER properties of MOF-derived layered double hydroxides (MLDH). By using multifunctional Ti3C2 MXene as support and post-treating MOF with an etching-coprecipitating process, the resultant CoFe MLDH/Ti3C2 exhibits prominent OER performance with ultralow overpotentials of only 170 and 238 mV to achieve the current density of 10 and 100 mA/cm2, respectively. In addition, the experimental and theoretical calculation results prove the strong electronic interaction between CoFe MLDH and Ti3C2 MXene could modulate the binding strength of intermediates for OER. This work gives a direction to prepare MOF-based efficient catalysts and enhance the intrinsic activity of (oxy)hydroxide-based catalysts.

MXene-induced electronic optimization of metal-organic framework-derived CoFe LDH nanosheet arrays for efficient oxygen evolution

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MXene-induced electronic optimization of metal-organic framework-derived CoFe LDH nanosheet arrays for efficient oxygen evolution