Tungsten carbides, featured by their Pt-like electronic structure, have long been advocated as potential replacements for the benchmark Pt-group catalysts in hydrogen evolution reaction. However, tungsten-carbide catalysts usually exhibit poor alkaline HER performance because of the sluggish hydrogen desorption behavior and possible corrosion problem of tungsten atoms by the produced hydroxyl intermediates. Herein, we report the synthesis of tungsten atomic clusters anchored on P-doped carbon materials via a thermal-migration strategy using tungsten single atoms as the parent material, which is evidenced to have the most favorable Pt-like electronic structure by in-situ variable-temperature near ambient pressure X-ray photoelectron spectroscopy measurements. Accordingly, tungsten atomic clusters show markedly enhanced alkaline HER activity with an ultralow overpotential of 53 mV at 10 mA/cm2 and a Tafel slope as low as 38 mV/dec. These findings may provide a feasible route towards the rational design of atomic-cluster catalysts with high alkaline hydrogen evolution activity.

The pursuit of selective two-electron oxygen reduction reaction to H2O2 in acids is demanding and largely hampered by the lack of efficient non-precious-metal-based electrocatalysts. Metal macrocycles hold promise, but have been relatively underexplored. Efforts are called for to promote their inherent catalytic activities and/or increase the surface exposure of active sites. In this contribution, we perform the high-throughput computational screening of thirty-two different metalloporphyrins by comparing their adsorption free energies towards key reaction intermediates. Cobalt porphyrin is revealed to be the optimal candidate with a theoretical overpotential as small as 40 mV. Guided by the computational predictions, we prepare hydrogen-bonded cobaltoporphyrin frameworks in order to promote the solution accessibility of catalytically active sites for H2O2 production in acids. The product features an onset potential at ~0.68 V, H2O2 selectivity of >90%, turnover frequency of 10.9 s−1 at 0.55 V and stability of ~30 h, the combination of which clearly renders it stand out from existing competitors for this challenging reaction.

Their nanoscale size endows perovskite quantum dots (QDs) with processing flexibility and high tunability of optoelectronic properties. The vast surface area also provides an opportunity for ligand engineering to offer QDs extra protection, which however, will impede charge transport in the QD array. Currently, the surface treatments that can balance both stability and conductivity of the perovskite QD array remain a huge challenge. Here, we report in situ growth of an atomic guanidinium lead iodide perovskite matrix on CsPbI 3 QDs. In addition to the effect of trap passivation, the matrix can also provide substantial surface strain to improve the QD phase stability. Meanwhile, the ultrathin matrix allows efficient coupling and charge transport in the QD solids. As a result, the CsPbI 3 QD solar cells can achieve both superior device stability and performance. We believe the development of a multifunctional surface matrix will become one of the future research focuses in perovskite QD-based devices.

Iridium oxide (IrO2) is the predominant electrocatalyst for the oxygen evolution reaction (OER), but its low efficiency and high cost limit its applications. In this work, we have developed a strategy by combination of high-throughput density functional theory (DFT) and machine learning (ML) techniques for material discovery on IrO2-based electrocatalysts with enhanced OER activity. A total of 36 kinds of metal dopants are considered to substitute for Ir to form binary and ternary metal oxides, and the most stable surface structures are selected from a total of 4648 structures for OER activity evaluation. Utilizing the neural network language model (NNLM), we associate the atomic environment with the formation energies of crystals and free energies of OER intermediates, and finally a series of potential candidates have been screened as the superior OER catalysts. Our strategy could efficiently explore promising electrocatalysts, especially for evaluating complex multi-metallic compounds.

In this work, we suggest SiS2 and SiSe2 as anode materials for sodium-ion batteries based on the first-principles prediction. Both SiS2 and SiSe2 have suitable adsorption energies (-1.01/-1.24 eV) and...