摘要
苯甲醛(BnCHO)作为制造染料的中间体,同时也是生产药品和香料等精细化工产品的重要原料,在精细化学合成中,利用光催化将苯甲醇氧化为苯甲醛具有潜在的应用前景.本研究将不同的金属离子(M=Fe,Co,Cu,Zn)固载于单缺位多金属氧酸盐[SiW11O39]8-(SiW),得到单金属取代多金属氧酸盐(MSiW),进而制备单分散多金属氧酸盐分子簇催化剂MSiW/CN.在不添加H2O2等额外氧化剂的情况下,利用MSiW/CN进行苯甲醇光氧化以制备苯甲醛.催化实验表明在12 h内,苯甲醇的转化率近乎达到69.17％,产率为532.13 mmol·g-1.与单纯的CN和FeSiW相比,苯甲醛的产量分别提高了 76倍和5倍,充分说明了光催化剂FeSiW/CN-7的优越性.5次循环后,FeSiW/CN-7仍保持较高的催化效率,表明其具有良好的催化稳定性.实验表明,所设计的FeSiW/CN-7能够在温和条件下利用光氧化制备苯甲醛,是一种极具前景的光催化剂.
Abstract
Benzaldehyde(BnCHO)is a key component in dye production and a fundamental substance in the fine chemical sector,especially for making medicines and flavorings.Under ambient conditions,the synthesis of BnCHO through the photo-oxidation of benzyl alcohol(BnOH)demonstrates significant ap-plication potential in fine chemical synthesis.Herein,we anchored different metal cations(M=Fe,Co,Cu,and Zn)into monolacunary polyoxometalate(POM)[SiW11O39]8-(SiW)to form single-metal substi-tuted-POMs(MSiWs).Furthermore,we have successfully dispersed these POMs uniformly onto poly-meric carbon nitride nanosheets(CN).For BnOH photooxidation without adding extra oxidants such as H2O2,the FeSiW/CN-7 exhibited excellent photocatalytic performance with the conversion of BnOH near-ly 69.17％and a BnCHO yield of 532.13 mmol·g-1 within 12 h.The photo-oxidation performance of BnOH is 76 and 5 times higher than that of single CN and FeSiW,respectively.This catalytic system can maintain a high catalytic efficiency after 5 cycles,indicating that FeSiW/CN possesses high catalytic stabil-ity.The results suggest that the designed POM-based single-atom catalyst FeSiW/CN is a promising can-didate for the preparation of BnCHO through photooxidation under mild conditions.
NETL
NSTL
万方数据