Photocatalytic Formic Acid Conversion on CdS Nanocrystals with Controllable Selectivity for H2 or CO
Photocatalytic Formic Acid Conversion on CdS Nanocrystals with Controllable Selectivity for H2 or CO
复制标题
DOI：
10.1002/anie.201502773
复制
发表时间：
2015-08-10
影响因子：
16.6
通讯作者：
Reisner, Erwin
中科院分区：
文献类型：
--
作者：
Kuehnel, Moritz F.;Wakerley, David W.;Reisner, Erwin
甲酸被认为是一种有前途的能量载体和储氢材料，用于碳中性经济。我们提出了一种廉价的系统，用于选择性的室温光催化转化甲酸为氢气或一氧化碳。在可见光照射下（> 420 nm，1 sun），配体包覆的硫化镉纳米晶体在甲酸/甲酸钠中的悬浮液释放高达116 +/-14 mmolH（2）g（cat）（-1）h（-1），当与钴助催化剂结合时，选择性>99%;在= 460 nm处的量子产率为21.2 +/-2.7%。在没有封端配体的情况下，相同的光催化剂在甲酸钠水溶液中的悬浮液产生高达102 +/-13 mmolCOg（cat）（-1）h（-1），选择性>95%，量子产率为19.7 +/- 2.7%。H-2和CO的生产持续了一周以上，周转数分别大于6x 10（5）和3x 10（6）。
Formic acid is considered a promising energy carrier and hydrogen storage material for a carbon-neutral economy. We present an inexpensive system for the selective room-temperature photocatalytic conversion of formic acid into either hydrogen or carbon monoxide. Under visible-light irradiation (>420nm, 1sun), suspensions of ligand-capped cadmium sulfide nanocrystals in formic acid/sodium formate release up to 116 +/- 14mmolH(2)g(cat)(-1)h(-1) with >99% selectivity when combined with a cobalt co-catalyst; the quantum yield at =460nm was 21.2 +/- 2.7%. In the absence of capping ligands, suspensions of the same photocatalyst in aqueous sodium formate generate up to 102 +/- 13mmolCOg(cat)(-1)h(-1) with >95% selectivity and 19.7 +/- 2.7% quantum yield. H-2 and CO production was sustained for more than one week with turnover numbers greater than 6x10(5) and 3x10(6), respectively.