AI Article Synopsis
- This paper presents a photocatalytic hydrogen evolution system that is responsive to surrounding pH levels, utilizing a microhydrogel matrix containing CdSe/CdS nanorods as photocatalysts.
- The microgel's actuation (swelling and contraction) happens quickly—within 0.58 to 1.7 seconds—and causes significant changes in the microgel's size and photocatalytic efficiency.
- Investigations reveal that the interaction between photoexcited holes and sulfite ions defines the system's pH responsiveness, as further detailed by molecular dynamics simulations.
Article Abstract
This paper describes a photocatalytic hydrogen evolution system that is dynamically and reversibly responsive to the pH of the surrounding solution through the actuation of a microhydrogel (microgel) matrix that hosts the photocatalysts (CdSe/CdS nanorods). The reversible actuation occurs within 0.58 (swelling) and 1.7 s (contraction). ΔpH = 0.01 relative to the p of the tertiary amine on the microgel polymer (7.27) results in a reversible change in the average diameter of the microgel hosts by a factor of 2.4 and a change in the photocatalytic turnover frequency (TOF) by a factor of 5. Kinetic isotope effect and photoluminescence quenching experiments reveal that the scavenging of the photoexcited hole by sulfite ions is the rate-limiting step and leads to the observed response of the TOF to pH through the actuation of the microgel. Molecular dynamics simulations quantify a greater local concentration of sulfite hole scavengers for pH < p.
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| http://dx.doi.org/10.1021/acs.jpclett.1c03713 | DOI Listing |
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