Dark Photocatalysis: Storage of Solar Energy in Carbon Nitride for Time-Delayed Hydrogen Generation

Vincent Wing hei Lau, Daniel Klose, Hatice Kasap, Filip Podjaski, Marie Claire Pignié, Erwin Reisner, Gunnar Jeschke, Bettina V. Lotsch

Research output: Contribution to journalArticlepeer-review

156 Citations (Scopus)

Abstract

While natural photosynthesis serves as the model system for efficient charge separation and decoupling of redox reactions, bio-inspired artificial systems typically lack applicability owing to synthetic challenges and structural complexity. We present herein a simple and inexpensive system that, under solar irradiation, forms highly reductive radicals in the presence of an electron donor, with lifetimes exceeding the diurnal cycle. This radical species is formed within a cyanamide-functionalized polymeric network of heptazine units and can give off its trapped electrons in the dark to yield H2, triggered by a co-catalyst, thus enabling the temporal decoupling of the light and dark reactions of photocatalytic hydrogen production through the radical′s longevity. The system introduced here thus demonstrates a new approach for storing sunlight as long-lived radicals, and provides the structural basis for designing photocatalysts with long-lived photo-induced states.

Original languageEnglish
Pages (from-to)510-514
Number of pages5
JournalAngewandte Chemie - International Edition
Volume56
Issue number2
DOIs
Publication statusPublished - 2017 Jan 9

All Science Journal Classification (ASJC) codes

  • Catalysis
  • Chemistry(all)

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