Self-Assembled Amphiphilic Molecules for Highly Efficient Photocatalytic Hydrogen Evolution from Water

Abstract

Self-assembled molecules for outstanding hydrogen evolution rate and durability should promise practical water splitting due to the versatile visible light absorption, low production cost, and ease of control. Here, we adapted an amphiphilic molecule as a building block for efficient small molecule based self-assembled photocatalyst for hydrogen evolution from water. The self-assembled molecules with platinum cocatalyst showed outstanding performance (turnover number ∼27000) virtually comparable to the state-of-the-art metal oxide based photocatalysts with catalytic activity extending over days. Transient absorption studies in combination with quantum chemical calculations revealed that elaborate excited state engineering of the molecules resulted in such high performance of hydrogen evolution from water. This study shows that the self-assembled amphiphilic molecules could pave the way to more economical and reproducible production of hydrogen from water.

Controlling Photocatalytic Activity by Self‐Assembly – Tuning Perylene Bisimide Photocatalysts for the Hydrogen Evolution Reaction

“…[3][4][5][6][7] PBIs are have been reported. [24] Often PBIs are designed for solubility in organic solvents but they can be dispersed in water using a range of suitable functional groups including oligoamines, oligo(ethylene oxide)s, charged species such as sulfonates and amino acids at the imide position (Figure 1). [10,25,26] Many amino acid functionalized PBIs have been reported and can form selfassembled structures in aqueous solution or form hydrogels depending on the exact conditions used.…”

Controlling Activity by Self-Assembly – Tuning Perylene Bisimide Photocatalysts for the Hydrogen Evolution Reaction

“…[16][17][18][19][20] Some of these systems use perylene mono or bis imides in a self-assembled state, but other self-assembled photocatalysts have been reported. 21 Often PBIs are designed for solubility in organic solvents but they can be dispersed in water using a range of suitable functional groups including oligoamines, oligo(ethylene oxide)s, charged species such as sulfonates and amino acids at the imide position ( Figure 1). 10,22,23 Many amino acid functionalised PBIs have been reported and can form self-assembled structures in aqueous solution or form hydrogels depending on the exact conditions used.…”

Long-lived excited states of platinum(ii)-porphyrins for highly efficient photocatalytic hydrogen evolution

“…Recently, the research on photocatalytic hydrogen evolution (PHE) has been developed very fast for the production of H 2 as a clean energy and renewable fuel that would reduce the consumption of fossil fuels and alleviate the global warming crisis. 6 To date, various photocatalysts based on transition metal complexes, [7][8][9][10][11][12] porous materials, 3,[13][14][15][16] metal suldes/ oxides, [17][18][19] organic and inorganic hybrids, 11,[20][21][22][23][24][25] organic molecules, [26][27][28][29] and porphyrins 5,[30][31][32][33][34][35][36] have been demonstrated for efficient PHE. Among them porphyrins received much more attention for PHE due to their strong light absorption in the UVvisible region and easily tailorable photophysical and redox properties by integrating different aromatic chromophores to the porphyrin ring and inserting different metals in the porphyrin ring.…”