Perovskite Oxides Toward Oxygen Evolution Reaction: Intellectual Design Strategies, Properties and Perspectives.

Developing electrochemical energy storage and conversion devices (e.g., water splitting, regenerative fuel cells and rechargeable metal-air batteries) driven by intermittent renewable energy sources holds a great potential to facilitate global energy transition and alleviate the associated environmental issues. However, the involved kinetically sluggish oxygen evolution reaction (OER) severely limits the entire reaction efficiency, thus designing high-performance materials toward efficient OER is of prime significance to remove this obstacle. Among various materials, cost-effective perovskite oxides have drawn particular attention due to their desirable catalytic activity, excellent stability and large reserves. To date, substantial efforts have been dedicated with varying degrees of success to promoting OER on perovskite oxides, which have generated multiple reviews from various perspectives, e.g., electronic structure modulation and heteroatom doping and various applications. Nonetheless, the reviews that comprehensively and systematically focus on the latest intellectual design strategies of perovskite oxides toward efficient OER are quite limited. To bridge the gap, this review thus emphatically concentrates on this very topic with broader coverages, more comparative discussions and deeper insights into the synthetic modulation, doping, surface engineering, structure mutation and hybrids. More specifically, this review elucidates, in details, the underlying causality between the being-tuned physiochemical properties [e.g., electronic structure, metal-oxygen (M-O) bonding configuration, adsorption capacity of oxygenated species and electrical conductivity] of the intellectually designed perovskite oxides and the resulting OER performances, coupled with perspectives and potential challenges on future research. It is our sincere hope for this review to provide the scientific community with more insights for developing advanced perovskite oxides with high OER catalytic efficiency and further stimulate more exciting applications.

Lithium recovery and solvent reuse from electrolyte of spent lithium-ion battery.

Great progresses have been made in recovering valuable metals or regenerating materials from spent lithium-ion batteries (LIBs), but how to treat the spent electrolyte and recover its valuable components economically are still a bottleneck. In this study, the volatile organic solvents (dimethyl carbonate (DMC) and diethyl carbonate (DEC)) in spent electrolyte were recycled through vacuum distillation based on thermodynamic analysis and reused for LIBs. The recovery efficiencies of DMC and DEC reach almost 100% and 79.40%, respectively, under the distillation temperature of 130 °C for 120 min. The prepared electrolyte by recovered DMC and DEC shows high discharge capacity and good cycle performance (discharge capacity retention is over 99% after 400 cycles at 1C) by Li/graphite battery. Moreover, lithium left in non-volatile components (ethylene carbonate (EC)) was recovered as lithium carbonate (purity is 92.45%) with a recovery efficiency of 86.93%. The proposed process sheds light on the comprehensive recycling of electrolyte from spent LIBs.

Controlling of Ni-Based Composites in Salt Melt Synthesis with High Sodium-Ion Storage Performance.

Owing to its fascinating properties (such as high theoretical specific capacity and considerable conductivity), nickel sulfide (NiS) was investigated comprehensively as an anode material in sodium-ion batteries. However, they still suffered from volume expansion and sluggish kinetics, resulting in serious cycle capabilities. Herein, through controlling the kind of molten salts (Na2SO4, NaCl, and Na2CO3) in salt melt synthesis (SMS), a series of NiS with an N, S-codoped carbon layer was successfully prepared, accompanied with different morphologies and structures (earthworm-like belts and triangular and spherical particles). Tailored by the ionic strength and viscosity of molten salts, the as-prepared samples displayed different crystallization behaviors, bringing about a difference in electrochemical performance. As earthworm-like NiS@C was explored as an anode material for SIBs, an initial capacity of 712.5 mAh g-1 at 0.5 A g-1 could be obtained, and it still kept 527.4 mAh g-1 after 100 cycles. Even at 2.0 A g-1, a capacity of 508.6 mAh g-1 could be achieved. Meanwhile, with the assistance of detailed kinetic analysis, the rapid diffusion behaviors of Na+ and redox reaction mechanisms of as-fabricated samples were proven for the enhanced electrochemical properties. Given this, this work is expected to provide a method for designing the morphology and structure of metal sulfides, while shedding light on the orientation of fabricating advanced electrode materials for SIBs.

Theory-Guided Modulation of Optimal Silver Nanoclusters toward Efficient CO2 Electroreduction.

Electrochemical CO2 reduction reaction (CO2RR), when powered with intermittent but renewable energies, holds an attractive potential to close the anthropogenic carbon cycle through efficiently converting the exorbitantly discharged CO2 to value-added fuels and/or chemicals and consequently reduce the greenhouse gas emission. Through systematically integrating the density functional theory calculations, the modeling statistics of various proportions of CO2RR-preferred electroactive sites, and the theoretical work function results, it is found that the crystallographically unambiguous Ag nanoclusters (NCs) hold a high possibility to enable an outstanding CO2RR performance, particularly at an optimal size of around 2 nm. Motivated by this, homogeneously well-distributed ultrasmall Ag NCs with an average size of ∼2 nm (2 nm Ag NCs) were thus synthesized to electrochemically promote CO2RR, and the results demonstrate that the 2 nm Ag NCs are able to achieve a significantly larger CO partial current density [j(CO)], an impressively higher CO Faraday efficiency of over 93.8%, and a lower onset overpotential (η) of 146 mV as well as a remarkably higher energy efficiency of 62.8% and a superior stability of 45 h as compared to Ag nanoparticles (Ag NPs) and bulk Ag. Both theoretical computations and experimental results clearly and persuasively demonstrate an impressive promotion effect of the crystallographically explicit atomic structure for electrochemically reducing CO2 to CO, which exemplifies a novel design approach to more benchmark metal-based platforms for advancing the practically large-scale CO2RR application.