No abstract

Electrocatalysts with single metal atoms as active sites have received increasing attention owing to their high atomic utilization efficiency and exotic catalytic activity and selectivity. This review aims to provide a comprehensive summary on the recent development of such single-atom electrocatalysts (SAECs) for various energy-conversion reactions. The discussion starts with an introduction of the different types of SAECs, followed by an overview of the synthetic methodologies to control the atomic dispersion of metal sites and atomically resolved characterization using state-of-the-art microscopic and spectroscopic techniques. In recognition of the extensive applications of SAECs, the electrocatalytic studies are dissected in terms of various important electrochemical reactions, including hydrogen evolution reaction (HER), oxygen evolution reaction (OER), oxygen reduction reaction (ORR), carbon dioxide reduction reaction (CO2RR), and nitrogen reduction reaction (NRR). Examples of SAECs are deliberated in each case in terms of their catalytic performance, structure−property relationships, and catalytic enhancement mechanisms. A perspective is provided at the end of each section about remaining challenges and opportunities for the development of SAECs for the targeted reaction.

No abstract

Ammonia is a critical component in fertilizers, pharmaceuticals, and fine chemicals and is an ideal, carbon-free fuel. Recently, lithium-mediated nitrogen reduction has proven to be a promising route for electrochemical ammonia synthesis at ambient conditions. In this work, we report a continuous-flow electrolyzer equipped with 25–square centimeter–effective area gas diffusion electrodes wherein nitrogen reduction is coupled with hydrogen oxidation. We show that the classical catalyst platinum is not stable for hydrogen oxidation in the organic electrolyte, but a platinum-gold alloy lowers the anode potential and avoids the decremental decomposition of the organic electrolyte. At optimal operating conditions, we achieve, at 1 bar, a faradaic efficiency for ammonia production of up to 61 ± 1% and an energy efficiency of 13 ± 1% at a current density of −6 milliamperes per square centimeter.

No abstract

The electrolysis of water is promising for hydrogen production. The development of high-performance and low-cost hydrogen evolution reaction (HER) electrocatalysts is particularly important for the wide application of water electrolyzers. Tuning the hydrogen binding energy (HBE) of materials is an effective way to optimize the HER electrocatalysts, particularly for applications in an acidic environment. Here, we report the discovery of a Pt-free combination, PdMoGaInNi, which has the HBE optimum, via computer-facilitated screening. As the exploratory example of the two-dimensional high-entropy alloy (HEA) for HER, the PdMoGaInNi HEA nanosheets were synthesized to realize the predicted Pt-free combination with optimal HBE. The PdMoGaInNi HEA nanosheets exhibit a high HER activity with low overpotentials of 13 mV at 10 mA cm–2, outperforming commercial Pd/C and Pt/C catalysts. Given the high entropy, lattice distortion, and sluggish diffusion effects of HEA, the PdMoGaInNi shows great long-term durability for at least 200 h in a proton exchange membrane water electrolyzer.

Aims: To evaluate the efficacy and safety of fibrin sealant in conjunctival autograft fixation in pterygium surgery. Methods: Prospective, comparative, interventional case series. 40 eyes of 40 patients with nasal primary pterygium, 24 male and 16 female, were enrolled. The patients were assigned to two groups and each contained 12 male and 8 female based on the pterygium area encroaching onto the cornea. In one group the conjunctival autograft was attached to the sclera with fibrin sealant and the other group with nylon 10–0 sutures. All the patients were followed up postoperatively on days 1, 3, 7 and 14 then at months 1, 2, 6 and 12. The main outcome measures included operating time, postoperative symptoms, graft success, recurrence rate and complications. Results: The average operating time was significantly shorter (p < 0.001) in the fibrin sealant group and fewer postoperative symptom complaints were received as well. By the end of 1-year follow-up, the recurrence rate was 5% in the fibrin sealant group and 10% in the suture group (p = 1.000), and there was no statistically significant difference in complications (p > 0.05) between the two groups. Conclusions: It is safe and effective to use fibrin sealant for conjunctival autograft fixation. This method causes much fewer postoperative symptoms and shortens surgery time significantly, and the long-term results are also favorable.

Scanning probe block copolymer lithography (SPBCL), in combination with density-functional theory (DFT), has been used to design and synthesize hydrogen evolution catalysts. DFT was used to calculate the hydrogen adsorption energy on a series of single-element, bimetallic, and trimetallic (Au, Pt, Ni, and Cu) substrates to provide leads that could be synthesized in the form of alloy or phase-separated particles via SPBCL. PtAuCu (18 nm, ∼1:1:1 stoichiometry) has been identified as a homogeneous alloy phase that behaves as an effective hydrogen evolution catalyst in acidic aqueous media, even when it is made in bulk form via solution phase methods. Significantly, the bulk-prepared PtAuCu/C nanocatalyst discovered via this process exhibits an activity seven times higher than that of the state-of-the-art commercial Pt/C catalyst (based upon Pt content). The advantage of using SPBCL in the discovery process is that one can uniformly make particles, each consisting of a uniform phase combination (e.g., all alloy or all phase-segregated species) at a fixed elemental ratio, an important consideration when working with polyelemental species where multiple phases may exist.