Smart photovoltaic windows represent a promising green technology featuring tunable transparency and electrical power generation under external stimuli to control the light transmission and manage the solar energy. Here, we demonstrate a thermochromic solar cell for smart photovoltaic window applications utilizing the structural phase transitions in inorganic halide perovskite caesium lead iodide/bromide. The solar cells undergo thermally-driven, moisture-mediated reversible transitions between a transparent non-perovskite phase (81.7% visible transparency) with low power output and a deeply coloured perovskite phase (35.4% visible transparency) with high power output. The inorganic perovskites exhibit tunable colours and transparencies, a peak device efficiency above 7%, and a phase transition temperature as low as 105 °C. We demonstrate excellent device stability over repeated phase transition cycles without colour fade or performance degradation. The photovoltaic windows showing both photoactivity and thermochromic features represent key stepping-stones for integration with buildings, automobiles, information displays, and potentially many other technologies.
Precise control of elemental configurations within multimetallic nanoparticles (NPs) could enable access to functional nanomaterials with significant performance benefits. This can be achieved down to the atomic level by the disorder-to-order transformation of individual NPs. Here, by systematically controlling the ordering degree, we show that the atomic ordering transformation, applied to AuCu NPs, activates them to perform as selective electrocatalysts for CO reduction. In contrast to the disordered alloy NP, which is catalytically active for hydrogen evolution, ordered AuCu NPs selectively converted CO to CO at faradaic efficiency reaching 80%. CO formation could be achieved with a reduction in overpotential of ∼200 mV, and catalytic turnover was enhanced by 3.2-fold. In comparison to those obtained with a pure gold catalyst, mass activities could be improved as well. Atomic-level structural investigations revealed three atomic gold layers over the intermetallic core to be sufficient for enhanced catalytic behavior, which is further supported by DFT analysis.
The surface and interfaces of heterogeneous catalysts are essential to their performance as they are often considered to be active sites for catalytic reactions. With the development of nanoscience, the ability to tune surface and interface of nanostructures has provided a versatile tool for the development and optimization of a heterogeneous catalyst. In this Review, we present the surface and interface control of nanoparticle catalysts in the context of oxygen reduction reaction (ORR), electrochemical CO2 reduction reaction (CO2 RR), and tandem catalysis in three sections. In the first section, we start with the activity of ORR on the nanoscale surface and then focus on the approaches to optimize the performance of Pt-based catalyst including using alloying, core–shell structure, and high surface area open structures. In the section of CO2 RR, where the surface composition of the catalysts plays a dominant role, we cover its reaction fundamentals and the performance of different nanosized metal catalysts. For tandem catalysis, where adjacent catalytic interfaces in a single nanostructure catalyze sequential reactions, we describe its concept and principle, catalyst synthesis methodology, and application in different reactions.
Conversion of carbon dioxide to C-C hydrocarbons is a major pursuit in clean energy research. Despite tremendous efforts, the lack of well-defined catalysts in which the spatial arrangement of interfaces is precisely controlled hinders the development of more efficient catalysts and in-depth understanding of reaction mechanisms. Herein, we utilized the strategy of tandem catalysis to develop a well-defined nanostructured catalyst CeO-Pt@mSiO-Co for converting CO to C-C hydrocarbons using two metal-oxide interfaces. C-C hydrocarbons are found to be produced with high (60%) selectivity, which is speculated to be the result of the two-step tandem process uniquely allowed by this catalyst. Namely, the Pt/CeO interface converts CO and H to CO, and on the neighboring Co/mSiO interface yields C-C hydrocarbons through a subsequent Fischer-Tropsch process. In addition, the catalysts show no obvious deactivation over 40 h. The successful production of C-C hydrocarbons via a tandem process on a rationally designed, structurally well-defined catalyst demonstrates the power of sophisticated structure control in designing nanostructured catalysts for multiple-step chemical conversions.
Promotion of C–C bonds is one of the key fundamental questions in the field of CO2 electroreduction. Much progress has occurred in developing bulk-derived Cu-based electrodes for CO2-to-multicarbons (CO2-to-C2+), especially in the widely studied class of high-surface-area “oxide-derived” copper. However, fundamental understanding into the structural characteristics responsible for efficient C–C formation is restricted by the intrinsic activity of these catalysts often being comparable to polycrystalline copper foil. By closely probing a Cu nanoparticle (NP) ensemble catalyst active for CO2-to-C2+, we show that bias-induced rapid fusion or “electrochemical scrambling” of Cu NPs creates disordered structures intrinsically active for low overpotential C2+ formation, exhibiting around sevenfold enhancement in C2+ turnover over crystalline Cu. Integrating ex situ, passivated ex situ, and in situ analyses reveals that the scrambled state exhibits several structural signatures: a distinct transition to single-crystal Cu2O cubes upon air exposure, low crystallinity upon passivation, and high mobility under bias. These findings suggest that disordered copper structures facilitate C–C bond formation from CO2 and that electrochemical nanocrystal scrambling is an avenue toward creating such catalysts.
We enclose octahedral silver nanocrystals (Ag NCs) in metal-organic frameworks (MOFs) to make mesoscopic constructs O(h)-nano-Ag⊂MOF in which the interface between the Ag and the MOF is pristine and the MOF is ordered (crystalline) and oriented on the Ag NCs. This is achieved by atomic layer deposition of aluminum oxide on Ag NCs and addition of a tetra-topic porphyrin-based linker, 4,4',4″,4‴-(porphyrin-5,10,15,20-tetrayl)tetrabenzoic acid (H4TCPP), to react with alumina and make MOF [Al2(OH)2TCPP] enclosures around Ag NCs. Alumina thickness is precisely controlled from 0.1 to 3 nm, thus allowing control of the MOF thickness from 10 to 50 nm. Electron microscopy and grazing angle X-ray diffraction confirm the order and orientation of the MOF by virtue of the porphyrin units being perpendicular to the planes of the Ag. We use surface-enhanced Raman spectroscopy to directly track the metalation process on the porphyrin and map the distribution of the metalated and unmetalated linkers on a single-nanoparticle level.
Reducing the diameter of silver nanowires has been proven to be an effective way to improve their optoelectronic performance by lessening light attenuation. The state-of-the-art silver nanowires are typically around 20 nm in diameter. Herein we report a modified polyol synthesis of silver nanowires with average diameters as thin as 13 nm and aspect ratios up to 3000. The success of this synthesis is based on the employment of benzoin-derived radicals in the polyol approach and does not require high-pressure conditions. The strong reducing power of radicals allows the reduction of silver precursors to occur at relatively low temperatures, wherein the lateral growth of silver nanowires is restrained because of efficient surface passivation. The optoelectronic performance of as-prepared 13 nm silver nanowires presents a sheet resistance of 28 Ω sq at a transmittance of 95% with a haze factor of ∼1.2%, comparable to that of commercial indium tin oxide (ITO).
Pt-based alloys have shown great promise as cathodic catalysts for cost-effective proton-exchange membrane fuel cells. Post-synthesis treatment has been recognized as a critical step to improve the catalytic performance of Pt-based alloys. Here, we present the effects of catalyst processing on the catalytic behavior of Pt-Ni nanoframe electrocatalysts in oxygen reduction reaction. The Pt-Ni nanoframes were made by corroding the Ni-rich phase from solid rhombic dodecahedral particles. A total of three different corrosion procedures were compared. Among them, electrochemical corrosion led to the highest initial specific activity (1.35 mA cm at 0.95 V versus reversible hydrogen electrode) by retaining more Ni in the nanoframes. However, the high activity gradually went down in a subsequent stability test due to continuous Ni loss and concomitant surface reconstruction. On the other hand, the best stability was achieved by a more-aggressive corrosion using oxidative nitric acid. Although the initial activity was compromised, this procedure imparted a less-defective surface, and thus, the specific activity dropped by only 7% over 30 000 potential cycles. These results indicate a delicate trade-off between the activity and stability of Pt-Ni nanoframe electrocatalysts. The obtained understanding of how to balance the activity-stability trade-off via catalyst processing can be generalized to other Pt-based alloys.
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