• Energy Research

AbstractColloidal nanocrystals combine size‐ and facet‐dependent properties with solution processing. They offer thus a compelling suite of materials for technological applications. Their size‐ and facet‐tunable features are studied in synthesis; however, to exploit their features in optoelectronic devices, it will be essential to translate control over size and facets from the colloid all the way to the film. Larger‐diameter colloidal quantum dots (CQDs) offer the attractive possibility of harvesting infrared (IR) solar energy beyond absorption of silicon photovoltaics. These CQDs exhibit facets (nonpolar (100)) undisplayed in small‐diameter CQDs; and the materials chemistry of smaller nanocrystals fails consequently to translate to materials for the short‐wavelength IR regime. A new colloidal management strategy targeting the passivation of both (100) and (111) facets is demonstrated using distinct choices of cations and anions. The approach leads to narrow‐bandgap CQDs with impressive colloidal stability and photoluminescence quantum yield. Photophysical studies confirm a reduction both in Stokes shift (≈47 meV) and Urbach tail (≈29 meV). This approach provides a ≈50% increase in the power conversion efficiency of IR photovoltaics compared to controls, and a ≈70% external quantum efficiency at their excitonic peak.

Solution-processed semiconductors are promising materials to realize optoelectronic devices that combine high performance with inexpensive manufacturing. In particular, the exploitation of colloidal quantum dots (CQDs) capable of harvesting infrared photons, in conjunction with visible-absorbing organic chromophores, has been demonstrated as an interesting route. Unfortunately, CQD/organic hybrid photovoltaics have been limited to power conversion efficiencies (PCEs) below 10% due to chemical mismatch and difficulties in facilitating charge collection. Here we devise a hybrid architecture that overcomes these limitations by introducing small molecules into the CQD/organic stacked structure. The small molecule complements CQD absorption and creates an exciton cascade with the host polymer, thus enabling efficient energy transfer and also promoting exciton dissociation at heterointerfaces. The resulting hybrid solar cells exhibit PCEs of 13.1% and retain over 80% of their initial PCE after 150 h of continuous operation unencapsulated, outperforming present air-processed solution-cast CQD/organic photovoltaics. Colloidal quantum dots and organics have complementary properties apt for photovoltaics, yet their combination has led to poor charge collection. Here, Baek et al. introduce small molecules that act as a bridge between quantum dots and polymers, thus improving device efficiency and stability.

Carbon dioxide/monoxide (CO2/CO) electrolysis provides a means to convert emissions into multicarbon products. However, impractical energy and carbon efficiencies limit current systems. Here we show that these inefficiencies originate from uncontrolled gas/ion distributions in the local reaction environment. Understanding of the flows of cations and anions motivated us to seek a route to block cation migration to the catalyst surface—a strategy we instantiate using a covalent organic framework (COF) in bulk heterojunction with a catalyst. The π-conjugated hydrophobic COFs constrain cation (potassium) diffusion via cation–π interactions, while promoting anion (hydroxide) and gaseous feedstock adsorption on the catalyst surface. As a result, a COF-mediated catalyst enables electrosynthesis of multicarbon products from CO for 200 h at a single-pass carbon efficiency of 95%, an energy efficiency of 40% and a current density of 240 mA cm−2. ; This work was financially supported by the Ontario Research Fund – Research Excellence programme, the Natural Sciences and Engineering Research Council (NSERC) of Canada and Natural Resources Canada’s Clean Growth Program. This research used synchrotron resources of the Advanced Photon Source (an Office of Science User Facility operated for the US Department of Energy (DOE) Office of Science by Argonne National Laboratory) and was supported by the US DOE under contract number DE-AC02-06CH11357, as well as the Canadian Light Source and its funding partners. Support from the Canada Research Chairs Program is gratefully acknowledged, as is support from an NSERC E.W.R. Steacie Fellowship to D.S. J.L. thanks the National Natural Science Foundation of China (grant number BE3250011), the National Key Research and Development Program of China (grant number 2022YFA1505100), and Shanghai Jiao Tong University (grant number WH220432516) for support. F.P.G.d.A. acknowledges funding from CEX2019-000910-S (MCIN/AEI/10.13039/501100011033), Fundación Cellex, Fundació Mir-Puig, Generalitat de ...

Colloidal quantum dot (CQD) materials are of interest in thin-film solar cells due to their size-tunable bandgap and low-cost solution-processing. However, CQD solar cells suffer from inefficient charge extraction over the film thicknesses required for complete absorption of solar light. Here we show a new strategy to enhance light absorption in CQD solar cells by nanostructuring the CQD film itself at the back interface. We use two-dimensional finite-difference time-domain (FDTD) simulations to study quantitatively the light absorption enhancement in nanostructured back interfaces in CQD solar cells. We implement this experimentally by demonstrating a nanoimprint-transfer-patterning (NTP) process for the fabrication of nanostructured CQD solids with highly ordered patterns. We show that this approach enables a boost in the power conversion efficiency in CQD solar cells primarily due to an increase in short-circuit current density as a result of enhanced absorption through light-trapping.

This research has been supported by Fundacio0 Privada Cellex Barcelona and the European Commission’s Seventh Framework Programme for Research under contract PIRG06-GA-2009-256355 and the Ministerio de Ciencia e Innovacion under Contract No. TEC2011-24744.

AbstractConstructing effective antidotes to reduce global health impacts induced by alcohol prevalence is a challenging topic. Despite the positive effects observed with intravenous applications of natural enzyme complexes, their insufficient activities and complicated usage often result in the accumulation of toxic acetaldehyde, which raises important clinical concerns, highlighting the pressing need for stable oral strategies. Here we present an effective solution for alcohol detoxification by employing a biomimetic-nanozyme amyloid hydrogel as an orally administered catalytic platform. We exploit amyloid fibrils derived from β-lactoglobulin, a readily accessible milk protein that is rich in coordinable nitrogen atoms, as a nanocarrier to stabilize atomically dispersed iron (ferrous-dominated). By emulating the coordination structure of the horseradish peroxidase enzyme, the single-site iron nanozyme demonstrates the capability to selectively catalyse alcohol oxidation into acetic acid, as opposed to the more toxic acetaldehyde. Administering the gelatinous nanozyme to mice suffering from alcohol intoxication significantly reduced their blood-alcohol levels (decreased by 55.8% 300 min post-alcohol intake) without causing additional acetaldehyde build-up. Our hydrogel further demonstrates a protective effect on the liver, while simultaneously mitigating intestinal damage and dysbiosis associated with chronic alcohol consumption, introducing a promising strategy in effective alcohol detoxification.

AbstractThe energy disorder that arises from colloidal quantum dot (CQD) polydispersity limits the open‐circuit voltage (VOC) and efficiency of CQD photovoltaics. This energy broadening is significantly deteriorated today during CQD ligand exchange and film assembly. Here, a new solution‐phase ligand exchange that, via judicious incorporation of reactivity‐engineered additives, provides improved monodispersity in final CQD films is reported. It has been found that increasing the concentration of the less reactive species prevents CQD fusion and etching. As a result, CQD solar cells with a VOC of 0.7 V (vs 0.61 V for the control) for CQD films with exciton peak at 1.28 eV and a power conversion efficiency of 10.9% (vs 10.1% for the control) is achieved.