Department of Chemistry, Collaborative Innovation Center of Chemical Science and Engineering, Nankai University, Tianjin 300071, People's Republic of China.
Dalton Trans. 2018 Sep 18;47(36):12726-12733. doi: 10.1039/c8dt02803f.
Two copper(ii)-based layered complexes with or without the amino group, [Cu(HL)2(NH2-BDC)]n (1) and [Cu(HL)2(BDC)]n (2) (HL = 4'-(4-hydroxyphenyl)-4,2':6',4''-terpyridine, NH2-H2BDC = 2-amino-1,4-benzenedicarboxylic acid and H2BDC = 1,4-benzenedicarboxylic acid), were solvothermally synthesized and used as photocatalysts to accelerate hydrogen production from water splitting. The amino group modified 1 has exhibited greatly enhanced photocatalytic activity with a hydrogen production rate of 2.34 mmol g-1 h-1 under visible light irradiation, which is almost double that of 2. Density functional theory calculations, electrochemical impedance spectroscopy and transient photocurrent tests demonstrate that the higher catalytic activity of 1 than 2 is a result of the enriched electron density around the CuII center by the amino group, which facilitates the charge transfer from the conduction band to the water molecule.
两个含有或不含有氨基的铜（II）层状配合物，[Cu(HL)2(NH2-BDC)]n (1) 和 [Cu(HL)2(BDC)]n (2) (HL = 4'-(4-羟基苯基)-4,2':6',4''-三联吡啶，NH2-H2BDC = 2-氨基-1,4-苯二甲酸，H2BDC = 1,4-苯二甲酸)，通过溶剂热法合成，并用作光催化剂，以加速水分解产生氢气。氨基修饰的 1 在可见光照射下具有显著增强的光催化活性，其氢气产生速率为 2.34 mmol g-1 h-1，几乎是 2 的两倍。密度泛函理论计算、电化学阻抗谱和瞬态光电流测试表明，1 比 2 具有更高的催化活性，是由于氨基周围 CuII 中心的电子密度增加，促进了从导带到水分子的电荷转移。
