期刊
ACS NANO
卷 15, 期 3, 页码 4226-4234出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.0c05992
关键词
spiky particles; electrocatalysis; colloids; noble-metal free; photooxidation; lignin
类别
资金
- NSF [1566460, 1463474, DMR-0315633, DMR-0320740]
- ONR [N000141812876]
- Vannewar Bush DoD Fellowship
- ONR Multidisciplinary University Research Initiative Award [N00014-18-1-2497]
- Direct For Mathematical & Physical Scien [1566460] Funding Source: National Science Foundation
- Division Of Chemistry [1566460] Funding Source: National Science Foundation
The research demonstrates that microscale hedgehog particles with semiconductor nanoscale spikes exhibit enhanced stability in high salt conditions, allowing for tuning of photocatalytic reactions by amplifying local electrical fields. This results in a significant increase in product yield in catalytic reactions.
High ionic strength environments can profoundly influence catalytic reactions involving charged species. However, control of selectivity and yield of heterogeneous catalytic reactions involving nano- and microscale colloids remains hypothetical because high ionic strength leads to aggregation of particle dispersions. Here we show that microscale hedgehog particles (HPs) with semiconductor nanoscale spikes display enhanced stability in solutions of monovalent/divalent salts in both aqueous and hydrophobic media. HPs enable tuning of photocatalytic reactions toward high-value products by adding concentrated inert salts to amplify local electrical fields in agreement with Derjaguin, Landau, Verwey, and Overbeek theory. After optimization of HP geometry for a model photocatalytic reaction, we show that high salt conditions increase the yield of HP-facilitated photooxidation of 2-phenoxy-1-phenylethanol to benzaldehyde and 2-phenoxyacetophenone by 6 and 35 times, respectively. Depending on salinity, electrical fields at the HP-media interface increase from 1.7 x 10(4) V/m to 8.5 x 10(7) V/m, with high fields favoring products generated via intermediate cation radicals rather than neutral species. Electron transfer rates were modulated by varying the ionic strength, which affords a convenient and hardly used reaction pathway for engineering a multitude of redox reactions including those involved in the environmental remediation of briny and salty water.
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