Photocatalytic anaerobic organic oxidation coupled with H2?evolution represents an advanced solar energy utilization strategy for the coproduction of clean fuel and fine chemicals. To achieve a high conversion efficiency, the smart design of efficient catalysts by the right combination of semiconductor light harvesters and cocatalyst is highly required. Herein, we report a composite photocatalyst composed of noble metal-free transition metal nitride Ni3FeN decorated on 2D ultrathin ZnIn2S4?(ZIS) nanosheets for selective oxidation of aromatic alcohols to aldehydes pairing with H2?production. In the composite, ultrathin ZIS serves as a light harvester that greatly shortens the diffusion length of photogenerated charges, while the metallic nitride Ni3FeN acts as an advanced cocatalyst which not only captures the photoelectrons generated from the ultrathin ZIS to promote the charge separation, but also provides active sites to lower the overpotential and accelerate the H2?reduction. The best photocatalytic performance is found on ZIS/1.5% M-Ni3FeN, which shows a H2?generation rate of 2427.9 ¦Ìmol g-1?h?1?and a benzaldehyde (BAD) production rate of 2460 ¦Ìmol g-1?h-1, about 7.8-fold as high as that of bare ZIS. This work is anticipated to endorse the exploration of?transition metal nitrides as high-performance cocatalysts to promote the coupled photocatalytic organic transformation and H2?production.

中文翻译：

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超薄 ZnIn2S4 纳米片负载的金属 Ni3FeN 用于光催化耦合选择性醇氧化和 H2 演化

光催化厌氧有机氧化与放氢相结合代表了一种先进的太阳能利用策略，用于联合生产清洁燃料和精细化学品。为了实现高转换效率，非常需要通过半导体光收集器和助催化剂的正确组合来智能设计高效催化剂。在此，我们报道了一种由装饰在二维超薄 ZnIn2S4?(ZIS) 纳米片上的不含贵金属的过渡金属氮化物 Ni3FeN 组成的复合光催化剂，用于将芳香醇选择性氧化为醛并与 H2? 产生配对。在复合材料中，超薄 ZIS 作为光收集器，大大缩短了光生电荷的扩散长度，而金属氮化物Ni3FeN作为一种先进的助催化剂，不仅可以捕获超薄ZIS产生的光电子以促进电荷分离，还可以提供活性位点以降低过电势并加速H2还原。ZIS/1.5% M-Ni3FeN 的光催化性能最好，其 H2? 生成率为 2427.9 μmol g-1?h?1?，苯甲醛 (BAD) 生成率为 2460 μmol g-1? h-1，约为裸 ZIS 的 7.8 倍。这项工作有望支持过渡金属氮化物作为高性能助催化剂的探索，以促进耦合光催化有机转化和 H2 生产。ZIS/1.5% M-Ni3FeN 的光催化性能最好，其 H2? 生成率为 2427.9 μmol g-1?h?1?，苯甲醛 (BAD) 生成率为 2460 μmol g-1? h-1，约为裸 ZIS 的 7.8 倍。这项工作有望支持过渡金属氮化物作为高性能助催化剂的探索，以促进耦合光催化有机转化和 H2 生产。ZIS/1.5% M-Ni3FeN 的光催化性能最好，其 H2? 生成率为 2427.9 μmol g-1?h?1?，苯甲醛 (BAD) 生成率为 2460 μmol g-1? h-1，约为裸 ZIS 的 7.8 倍。这项工作有望支持过渡金属氮化物作为高性能助催化剂的探索，以促进耦合光催化有机转化和 H2 生产。