Bottom-up evolution of perovskite clusters into high-activity rhodium nanoparticles toward alkaline hydrogen evolution.

Self-reconstruction has been considered an efficient means to prepare efficient electrocatalysts in various energy transformation process for bond activation and breaking. However, developing nano-sized electrocatalysts through complete in-situ reconstruction with improved activity remains challenging. Herein, we report a bottom-up evolution route of electrochemically reducing CsRhI halide-perovskite clusters on N-doped carbon to prepare ultrafine Rh nanoparticles (~2.

Spin engineering of single-site metal catalysts.

Single-site metal atoms (SMAs) on supports are attracting extensive interest as new catalytic systems because of maximized atom utilization and superior performance. However, rational design of configuration-optimized SMAs with high activity from the perspectives of fundamental electron spin is highly challenging. Herein, N-coordinated Fe single atoms are successfully distributed over axial carbon micropores to form dangling-FeN centers (d-FeN).

Caged-Cation-Induced Lattice Distortion in Bronze TiO for Cohering Nanoparticulate Hydrogen Evolution Electrocatalysts.

Defect engineering provides a promising approach for optimizing the trade-off between support structures and active nanoparticles in heterojunction nanostructures, manifesting efficient synergy in advanced catalysis. Herein, a high density of distorted lattices and defects are successfully formed in bronze TiO through caging alkali-metal Na cations in open voids (Na-TiO(B)), which could efficiently cohere nanoparticulate electrocatalysts toward alkaline hydrogen evolution reaction (HER). The RuMo bimetallic nanoparticles could directionally anchor on Na-TiO(B) with a certain angle of ∼22° due to elimination of the lattice mismatch, thus promoting uniform dispersion and small sizing of supported nanoparticles.

Intrinsic Electron Localization of Metastable MoS Boosts Electrocatalytic Nitrogen Reduction to Ammonia.

The advancement of efficient electrocatalysts toward the nitrogen reduction reaction (NRR) is critical in sustainable ammonia synthesis under ambient pressure and temperature. Manipulating the electronic configuration of electrocatalysts is particularly vital to form metal-nitrogen (MN) bonds during the NRR through regulating the active electronic states of sites. Here, in sharp contrast to stable 2H MoS without metal chains, MoMo bonding in metastable polymorphs of MoS bulk (zigzag chain in the 1T' phase and diamond chain in the 1T″' phase) is discovered to significantly increase intrinsic electron localization around the metal chains.

Interface Engineering with Ultralow Ruthenium Loading for Efficient Water Splitting.

Developing high-performance and cost-effective bifunctional electrocatalysts for water splitting is the key to large-scale hydrogen production. How to achieve higher performance with a lower amount of noble metal is still a major challenge. Herein, using a facile wet-chemistry strategy, we report the ultralow amount loading of ruthenium (Ru) on porous nickel foam (NF) as a highly efficient bifunctional electrocatalyst for water splitting.