CdS quantum dot aerogels for photocatalytic hydrogen evolution

IF 9 2区 材料科学 Q1 CHEMISTRY, PHYSICAL
Vinicius Alevato, Daniel Streater, Cole Premtaj, Jier Huang, Stephanie L. Brock
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Abstract

CdS quantum dots (QDs) have been extensively studied as photocatalysts and sensitizers for visible-light-driven water reduction. However, their efficiencies are limited by the need to accumulate sufficient redox equivalents to produce H2 and consequent photocorrosion associated with slow hole-transfer rates. To address these limitations, we report the formation of CdS QD assemblies (aerogels, AGs) capable of facilitating energy/charge transport between individual QDs, and evaluate their performance as photocatalysts for hydrogen evolution as a function of structure, wurtzite (w-) vs. zincblende (zb-), and different annealing temperatures. The formation of AGs from QDs resulted in increased rates of H2 production under visible light illumination: from 1458 (QD) to 6650 (AG) µmolH2·h−1·g−1 on zbCdS and from 1221 (QD) to 3325 (AG) µmolH2·h−1·g−1 on wCdS. This is attributed to exciton delocalization between adjacent QDs facilitating charge/energy transport. Thermal processing of CdS AGs up to 250 °C improved their activity, increasing the degree of exciton delocalization, while annealing them to 300 °C caused sintering of the primary QD particles within the AGs and a decrease in activity associated with loss in surface area. The best photocatalyst, zbCdS AG annealed at 250°C, had an average H2 production rate of 13,604 ± 2017 µmolH2·h−1·g−1, an apparent quantum yield of 2.8% at 425 ± 12.5 nm, and was stable for 2 h before beginning to deactivate due to photocorrosion. This study confirms the potential of CdS AGs as matrixes for the design of more active and stable composite photocatalysts for water splitting.

光催化析氢用CdS量子点气凝胶
CdS量子点(QDs)作为可见光驱动水还原的光催化剂和敏化剂得到了广泛的研究。然而,它们的效率受到需要积累足够的氧化还原当量来产生H2和随之而来的光腐蚀(与缓慢的空穴转移速率相关)的限制。为了解决这些限制,我们报道了能够促进单个量子点之间能量/电荷传输的CdS量子点组装(气凝胶,AGs)的形成,并评估了它们作为析氢光催化剂的性能,作为结构的函数,紫锌矿(w-)与锌闪锌矿(zb-),以及不同的退火温度。在可见光照射下,由量子点形成的AGs增加了H2的产率:zbcd从1458 (QD)增加到6650 (AG)µmolH2·h−1·g−1,wcd从1221 (QD)增加到3325 (AG)µmolH2·h−1·g−1。这是由于相邻量子点之间的激子离域促进了电荷/能量输运。在250°C下对CdS AGs进行热处理,提高了它们的活性,增加了激子离域的程度,而在300°C下退火会导致AGs内部的初级量子点颗粒烧结,并且活性降低,这与表面积损失有关。250℃退火zbCdS AG的平均产氢速率为13604±2017µmolH2·h−1·g−1,在425±12.5 nm处的表观量子产率为2.8%,且稳定2 h后开始因光腐蚀失活。该研究证实了CdS - AGs作为设计更活跃、更稳定的水裂解复合光催化剂的基质的潜力。
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来源期刊
Nano Research
Nano Research 化学-材料科学:综合
CiteScore
14.30
自引率
11.10%
发文量
2574
审稿时长
1.7 months
期刊介绍: Nano Research is a peer-reviewed, international and interdisciplinary research journal that focuses on all aspects of nanoscience and nanotechnology. It solicits submissions in various topical areas, from basic aspects of nanoscale materials to practical applications. The journal publishes articles on synthesis, characterization, and manipulation of nanomaterials; nanoscale physics, electrical transport, and quantum physics; scanning probe microscopy and spectroscopy; nanofluidics; nanosensors; nanoelectronics and molecular electronics; nano-optics, nano-optoelectronics, and nano-photonics; nanomagnetics; nanobiotechnology and nanomedicine; and nanoscale modeling and simulations. Nano Research offers readers a combination of authoritative and comprehensive Reviews, original cutting-edge research in Communication and Full Paper formats. The journal also prioritizes rapid review to ensure prompt publication.
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