The wide spectral range of the solar flux with undesirable diffused energy distribution remains a substantial impediment to the high-efficiency utilization of the whole spectrum. Here, inspired by the spectrally selective sunlight utilization of plants, a spectrum-tailored solar harnessing aerogel is conceived. It is composed of oxygen vacancy (O v) defect-rich semiconductor HNb 3 O 8 (D-HNb 3 O 8) nanosheets and polyacrylamide (PAM) framework to perform all-in-one photochemical and photothermal full solar energy conversion. The aerogel selectively utilizes the whole solar spectrum, in which high energy ultraviolet (UV) photon is converted into high redox potential electron-hole pairs, while low energy visible-near infrared (NIR) photons are transformed into heat. The designed solar absorber-polymer composite shows energy harnessing-conversion capability with desired heat insulation, reactant enrichment, rapid mass diffusion and capillary pumping characteristics, thus realizing a high efficient steam generation and photochemical activity. This cooperative photochemical and photothermal solar energy conversion, at respective optimal working spectrum, holds great promise for optimizing and maximizing the solar energy utilization, as well as opening up opportunities to explore simultaneous multifunctional usage of solar energy.
Triboelectric nanogenerators with enhanced output performance by surface texturing and dielectric constant control.
Lithium carbonate plays a critical role in both lithium-carbon dioxide and lithium-air batteries as the main discharge product and a product of side reactions, respectively. Understanding the decomposition of lithium carbonate during electrochemical oxidation (during battery charging) is key for improving both chemistries, but the decomposition mechanisms and the role of the carbon substrate remain under debate. Here, we use an in-situ differential electrochemical mass spectrometry-gas chromatography coupling system to quantify the gas evolution during the electrochemical oxidation of lithium carbonate on carbon substrates. Our results show that lithium carbonate decomposes to carbon dioxide and singlet oxygen mainly via an electrochemical process instead of via a chemical process in an electrolyte of lithium bis(trifluoromethanesulfonyl)imide in tetraglyme. Singlet oxygen attacks the carbon substrate and electrolyte to form both carbon dioxide and carbon monoxide—approximately 20% of the net gas evolved originates from these side reactions. Additionally, we show that cobalt(II,III) oxide, a typical oxygen evolution catalyst, stabilizes the precursor of singlet oxygen, thus inhibiting the formation of singlet oxygen and consequent side reactions.
A significant methodology gap remains in the construction of advanced electrocatalysts, which has collaborative defective functionalities and structural coherence that maximizes electrochemical redox activity, electrical conductivity, and mass transport characteristics. Here, a coordinative self‐templated pseudomorphic transformation of an interpenetrated metal organic compound network is conceptualized into a defect‐rich porous framework that delivers highly reactive and durable photo(electro)chemical energy conversion functionalities. The coordinative‐template approach enables previously inaccessible synthesis routes to rationally accomplish an interconnected porous conductive network at the microscopic level, while exposing copious unsaturated reactive sites at the atomic level without electronic or structural integrity trade‐offs. Consequently, porous framework, interconnected motifs, and engineered defects endow remarkable electrocatalytic hydrogen evolution reaction and oxygen evolution reaction activity due to intrinsically improved turnover frequency, electrochemical surface area, and charge transfer. Moreover, when the hybrid is coupled with a silicon photocathode for solar‐driven water splitting, it enables photon assisted redox reactions, improved charge separation, and enhanced carrier transport via the built‐in heterojunction and additive co‐catalyst functionality, leading to a promising photo(electro)chemical hydrogen generation performance. This work signifies a viable and generic approach to prepare other functional interconnected metal organic coordinated compounds, which can be exploited for diverse energy storage, conversion, or environmental applications.
Solar energy represents a robust and natural form of resource for environment remediation via photocatalytic pollutant degradation with minimum associated costs. However, due to the complexity of the photodegradation process, it has been a long-standing challenge to develop reliable photocatalytic systems with low recombination rates, excellent recyclability, and high utilization rates of solar energy, especially in the visible light range. In this work, a ternary hetero-nanostructured Ag-CuO-ZnO nanotube (NT) composite is fabricated via facile and low-temperature chemical and photochemical deposition methods. Under visible light irradiation, the as-synthesized ZnO NT based ternary composite exhibits a greater enhancement (∼300%) of photocatalytic activity than its counterpart, Ag-CuO-ZnO nanorods (NRs), in pollutant degradation. The enhanced photocatalytic capability is primarily attributed to the intensified visible light harvesting, efficient charge carrier separation and much larger surface area. Furthermore, our as-synthesised hybrid ternary Ag-CuO-ZnO NT composite demonstrates much higher photostability and retains ∼98% of degradation efficiency even after 20 usage cycles, which can be mainly ascribed to the more stable polar planes of ZnO NTs than those of ZnO NRs. These results afford a new route to construct ternary heterostructured composites with perdurable performance in sewage treatment and photocorrosion suppression.
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