Gradient OH Desorption Facilitating Alkaline Hydrogen Evolution Over Ultrafine Quinary Nanoalloy

Advanced Energy Materials, Год журнала: 2024, Номер 14(25)

Опубликована: Апрель 5, 2024

Abstract Strengthening OH adsorption on electrocatalyst is crucial to promote the rate‐determining water dissociation step of alkaline hydrogen evolution reaction (HER), whereas too‐intensified will poison active sites instead. This dilemma remains one major challenges for improving electrocatalysts’ HER activities. Herein, a surprising finding that strongly adsorbed an ultrafine quinary PtCoCuNiZn nanoalloy can be facilely desorbed via unique gradient desorption pattern reported, which tremendously boosts its activity. Theoretical simulations unravel possesses versatile metal adsorbing and gradiently transferred desorb from with moderate energy barriers each transfer desorption. In meanwhile, mode also experimentally evidenced by in situ Raman spectroscopy cyclic voltammetry measurements. offers fresh opportunity expedite without compromising strength electrocatalysts, thus maximally promotes their properties unlocks full potential

Язык: Английский

---

Ultradurable Pt-Based Catalysts for Oxygen Reduction Electrocatalysis

Catalysts, Год журнала: 2024, Номер 14(1), С. 57 - 57

Опубликована: Янв. 12, 2024

An oxygen reduction reaction (ORR) is the key half of proton exchange membrane fuel cells (PEMFCs), and highly dependent on Pt-based nanocrystals as core electrocatalysts. Despite exceptional ORR activity from adjusting electronic structures surface or near-surface atoms, several serious issues, including corrosion carbon supports, preferential leaching active metal elements, instability low-coordinated atoms sintering/agglomeration nanocrystals, still exist, challenging durability developed catalysts. From point view catalyst structure design, in this review, we summarized state-of-the-art structural regulation strategies for improving The current limitation binary catalysts electrocatalysis firstly discussed, detailed are further classified into optimization metal-doped alloys, core/shell structures, intermetallics high-entropy etc. structure–performance relationship detailedly explained, especially emphasizing elimination above restrictions. Finally, existing challenges future research direction presented, aiming at practicing PEMFC devices ultradurable

Язык: Английский

---

Single‐Atom Titanium on Mesoporous Nitrogen, Oxygen‐Doped Carbon for Efficient Photo‐thermal Catalytic CO₂ Cycloaddition by a Radical Mechanism

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(23)

Опубликована: Апрель 6, 2024

Abstract Developing efficient and earth‐abundant catalysts for CO 2 fixation to high value‐added chemicals is meaningful but challenging. Styrene carbonate has great market value, the cycloaddition of styrene oxide difficult due steric hindrance weak electron‐withdrawing ability phenyl group. To utilize clean energy (such as optical energy) directly effectively process, we introduce Ti single‐atom into mesoporous nitrogen, oxygen‐doped carbon nanosheets (Ti−CNO) by a two‐step method. The Ti−CNO exhibits excellent photothermal catalytic activities stability carbonate. Under light irradiation ambient pressure, an optimal produces with yield 98.3 %, much higher than CN (27.1 %). In addition, it shows remarkable during 10 consecutive cycles. Its enhanced performance stems from effect improved Lewis acidic/basic sites exposed abundant mesopores. experiments theoretical simulations demonstrate oxide⋅ + ⋅ − radicals generated at acidic (Ti δ+ ) basic under irradiation, respectively. This work furnishes strategy synthesizing advanced photo‐thermal synergistic value products via pathway.

Язык: Английский

---

Investigation of the Relationship between Metal Loading and Acidic Oxygen Evolution Reaction Activity in Single-Atom Catalysts

ACS Catalysis, Год журнала: 2024, Номер 14(6), С. 3788 - 3797

Опубликована: Фев. 22, 2024

Revealing the underlying relationship between loading of metal atoms and catalytic behavior is crucial for guiding design optimal single-atom catalysts (SACs) in heterogeneous catalysis. However, apparent controlled by interactions individual active sites remains elusive. Here, we successfully synthesized a series atomically dispersed Ir SACs with Ir-PN3 configuration through straightforward P atom anchoring strategy, which effectively prevents aggregation due to its strong metal-coordination capabilities. These are loaded at varying percentages, ranging from 5% 21 wt %, exhibited an unforeseen "volcano-type" loadings their acidic oxygen evolution reaction activity. Notably, highest activity observed moderate level 14%. This phenomenon can be attributed competition number electronic structure sites. Electronic structural characterizations theoretical calculations reveal that key establishing among high densities, leading charge rearrangement. study highlights importance SACs, may not exhibit positive linear regression.

Язык: Английский

---

Advanced carbon nitride‐based single‐atom photocatalysts

SusMat, Год журнала: 2024, Номер 4(5)

Опубликована: Июль 18, 2024

Abstract Single‐atom catalysts (SACs) have rapidly become a hot topic in photocatalytic research due to their unique physical and chemical properties, high activity, selectivity. Among many semiconductor carriers, the special structure of carbon nitride (C 3 N 4 ) perfectly meets substrate requirements for stabilizing SACs; they can also compensate defects C materials by modifying energy bands electronic structures. Therefore, developing advanced ‐based SACs is great significance. In this review, we focus on elucidating efficient preparation strategies burgeoning applications SACs. We outline prospective enhancing performance future. A comprehensive array methodologies presented identifying characterizing This includes an exploration potential atomic catalytic mechanisms through simulation regulation behaviors synergistic effects single or multiple sites. Subsequently, forward‐looking perspective adopted contemplate future prospects challenges associated with encompasses considerations, such as loading, regulatory design, integration machine learning techniques. It anticipated that review will stimulate novel insights into synthesis high‐load durable SACs, thereby providing theoretical groundwork scalable controllable field.

Язык: Английский

---