ABSTRACT
Intensive research in electrochemical CO2 reduction reaction has resulted in the discovery of numerous high-performance catalysts selective to multi-carbon products, with most of these catalysts still being purely transition metal based. Herein, we present high and stable multi-carbon products selectivity of up to 76.6% across a wide potential range of 1 V on histidine-functionalised Cu. In-situ Raman and density functional theory calculations revealed alternative reaction pathways that involve direct interactions between adsorbed histidine and CO2 reduction intermediates at more cathodic potentials. Strikingly, we found that the yield of multi-carbon products is closely correlated to the surface charge on the catalyst surface, quantified by a pulsed voltammetry-based technique which proved reliable even at very cathodic potentials. We ascribe the surface charge to the population density of adsorbed species on the catalyst surface, which may be exploited as a powerful tool to explain CO2 reduction activity and as a proxy for future catalyst discovery, including organic-inorganic hybrids.
Subject(s)
Carbon Dioxide , Plastic Surgery Procedures , Histidine , Carbon , ElectrodesABSTRACT
Conjugated polymers are promising materials for thermoelectrics as they offer good performances at near ambient temperatures. The current focus on polymer thermoelectric research mainly targets a higher power factor (PF; a product of the conductivity and square of the Seebeck coefficient) through improving the charge mobility. This is usually accomplished via structural modification in conjugated polymers using different processing techniques and doping. As a result, the structure-charge transport relationship in conjugated polymers is generally well-established. In contrast, the relationship between the structure and the Seebeck coefficient is poorly understood due to its complex nature. A theoretical framework by David Emin (Phys. Rev. B, 1999, 59, 6205-6210) suggests that the Seebeck coefficient can be enhanced via carrier-induced vibrational softening, whose magnitude is governed by the size of the polaron. In this work, we seek to unravel this relationship in conjugated polymers using a series of highly identical pro-quinoid polymers. These polymers are ideal to test Emin's framework experimentally as the quinoid character and polaron delocalization in these polymers can be well controlled even by small atomic differences (<10 at. % per repeating unit). By increasing the polaron delocalization, that is, the polaron size, we demonstrate that both the conductivity and the Seebeck coefficient (and hence PF) can be increased simultaneously, and the latter is due to the increase in the polaron's vibrational entropy. By using literature data, we also show that this phenomenon can be observed in two closely related diketopyrrolopyrrole-conjugated polymers as well as in p-doped P3HT and PANI systems with an increasing molecular order.
ABSTRACT
In the present study, a convenient and highly efficient method was developed to quantify aflatoxin B1 (AFB1) in oil samples. Low temperature clean-up (LTC) followed by immuno magnetic solid phase extraction (IMSPE) was used to clean up oil samples. LTC assisted in freezing out the interference from the oil matrix while IMSPE further helped to preconcentrate the targeted analyte. For IMSPE, we synthesised and characterised anti-AFB1 monoclonal antibody-functionalised magnetic nanoparticles. Oil sample extraction was then carried out using LTC-IMSPE. The proposed method showed satisfactory efficiency and reproducibility with recovery rates being within the range of 79.6-117.9%, with a relative standard deviation below 11.48%. The sensitivity of the method was satisfactory with the limits of detection and quantification being as low as 0.0048 and 0.0126â¯ng·g-1, respectively. Real sample analysis was carried out for five kinds of different vegetable oils. The results suggest that the method developed is very sensitive and accurate.