A single-atom Pt 1 /CeO 2 catalyst formed by atom trapping (AT, 800 °C in air) shows excellent thermal stability but is inactive for CO oxidation at low temperatures owing to over-stabilization of Pt 2+ in a high...
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A single-atom Pt 1 /CeO 2 catalyst formed by atom trapping (AT, 800 °C in air) shows excellent thermal stability but is inactive for CO oxidation at low temperatures owing to over-stabilization of Pt 2+ in a highly symmetric square-planar Pt 1 O 4 coordination environment. Reductive activation to form Pt nanoparticles (NPs) results in enhanced activity; however, the NPs are easily oxidized, leading to drastic activity loss. Herein we show that tailoring the local environment of isolated Pt 2+ by thermal-shock (TS) synthesis leads to a highly active and thermally stable Pt 1 /CeO 2 catalyst. Ultrafast shockwaves (>1200 °C) in an inert atmosphere induced surface reconstruction of CeO 2 to generate Pt single atoms in an asymmetric Pt 1 O 4 configuration. Owing to this unique coordination, Pt 1 δ+ in a partially reduced state dynamically evolves during CO oxidation, resulting in exceptional low-temperature performance. CO oxidation reactivity on the Pt 1 /CeO 2 _TS catalyst was retained under oxidizing conditions.
Three-dimensionally ordered macroporous (3DOM) materials have aroused tremendous interest in solar light to energy conversion, sustainable and renewable products generation, and energy storage fields owing to their co...
Three-dimensionally ordered macroporous (3DOM) materials have aroused tremendous interest in solar light to energy conversion, sustainable and renewable products generation, and energy storage fields owing to their convenient mass transfer channels, high surface area, enhanced interaction between matter and light, plentiful reactive sites as well as tunable composition. In this review, the state-of-the-art 3DOM materials as well as their preparation methods and the relevant applications including photo/electrocatalytic sustainable energy conversion, solar cells, Li ion batteries and supercapacitor are thoroughly outlined. Meanwhile, the unique merits and mechanisms for 3DOM materials in various applications are revealed and discussed in depth. Moreover, the strategies for designing 3DOM materials and the enhanced performance for applications are correlated, which can be significantly valuable to help readers to promptly acquire the comprehensive knowledge and to inspire some new ideas in developing 3DOM materials for further improved performances. Finally, the challenges and perspectives of 3DOM materials for sustainable energy conversion/production, solar cells and energy storage fields are outlooked. We sincerely look forward to that this critical review can facilitate the fast developments in designing highly efficient 3DOM materials and the relevant applications.
The power conversion efficiencies (PCEs) of perovskite solar cells have recently developed rapidly compared to crystalline silicon solar cells. To have an effective way to control the crystallization of perovskite thi...
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The power conversion efficiencies (PCEs) of perovskite solar cells have recently developed rapidly compared to crystalline silicon solar cells. To have an effective way to control the crystallization of perovskite thin films is the key for achieving good device performance. However, a paradox in perovskite crystallization is from the mismatch between nucleation and Oswald ripening. Usually, the large numbers of nucleation sites tend to weak Oswald ripening. Here, we proposed a new mechanism to promote the formation of nucleation sites by reducing surface energy from 44.9 mN/m to 36.1 mN/m, to spontaneously accelerate the later Oswald ripening process by improving the grain solubility through the elastic modulus regulation. The ripening rate is increased from 2.37 Åm ⋅ s −1 to 4.61 Åm ⋅ s −1 during annealing. Finally, the solar cells derived from the optimized films showed significantly improved PCE from 23.14 % to 25.32 %. The long-term stability tests show excellent thermal stability (the optimized device without encapsulation maintaining 82 % of its initial PCE after 800 h aging at 85 °C) and an improved light stability under illumination. This work provides a new method, the elastic modulus regulation, to enhance the ripening process.
Die bemerkenswerte Allotropie von Kohlenstoff liefert zahlreiche topologisch mögliche Käfigstrukturen von molekularem Kohlenstoff. Dazu gehören auch die sogenannten endohedralen Metallofullerene, bei de...
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Die bemerkenswerte Allotropie von Kohlenstoff liefert zahlreiche topologisch mögliche Käfigstrukturen von molekularem Kohlenstoff. Dazu gehören auch die sogenannten endohedralen Metallofullerene, bei denen ein Metallatom im Käfig eingeschlossen ist. Stabile und lösliche leere Fullerene und endohedrale Metallofullerene in reiner Form sind in makroskopischen Mengen durch Erzeugung im Kohlenstofflichtbogen oder andere physikalische Prozesse mit anschließender Extraktion und chromatographischer Trennung verfügbar. Jedoch bleiben viele andere, nicht identifizierte Fulleren‐Spezies, die in ihrer reinen Form offenbar reaktiv und unlöslich sind, im Ruß zurück. Solche “fehlenden” Spezies müssen extrem kleine HOMO‐LUMO‐Aufspaltungen aufweisen und könnten unkonventionelle Käfigstrukturen zeigen. Jüngste Fortschritte in diesem Bereich haben gezeigt, dass sich reaktive Fullerene unter Verwendung einer exohedralen Derivatisierung gewinnen lassen, durch die die reaktiven Kohlenstoffkäfige stabilisiert werden können. Dieses Konzept bietet ein Mittel zur Produktion von makroskopischen Mengen unkonventioneller Fullerene.
The photoelectrochemical reduction of nitrate to ammonia (PEC NO 3 RR) has emerged as a promising pathway for facilitating the natural nitrogen cycle. The PEC NO 3 RR can lower the reduction potential needed for ammon...
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The photoelectrochemical reduction of nitrate to ammonia (PEC NO 3 RR) has emerged as a promising pathway for facilitating the natural nitrogen cycle. The PEC NO 3 RR can lower the reduction potential needed for ammonia synthesis through photogenerated voltage, showcasing the significant potential for merging abundant solar energy with sustainable nitrogen fixation. However, it is influenced by the selective photocathodes with poor carrier kinetics, low catalytic selectivity, and ammonia yields. There are few reports on suitable photoelectrodes owning efficient charge transport on PEC NO 3 RR at low overpotentials. Herein, we rationally constructed the CuSn alloy co-catalysts on the antimony sulfides with a highly selective PEC ammonia and an ultra-low onset potential (0.62 V RHE ). CuSn/TiO 2 /Sb 2 S 3 photoelectrodes achieved an ammonia faradic efficiency of 97.82 % at a low applied potential of 0.4 V RHE , and an ammonia yield of 16.96 μmol h −1 cm −2 at 0 V RHE under one sun illumination. Dynamics experiments and theoretical calculations have demonstrated that CuSn/TiO 2 /Sb 2 S 3 has an enhanced charge separation and transfer efficiency, facilitating photogenerated electrons to participate in PEC NO 3 RR quickly. Meanwhile, moderate NO 2 * adsorption on this photocathode optimizes the catalytic activity and increases the NH 4 + yield. This work opens an avenue for designing sulfide-based photocathodes for the efficient route of solar-to-ammonia conversion.
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