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Fragmentation of supported gold nanoparticles@agarose film by thiols and the role of their synergy in efficient catalysis

机译:巯基对负载的金纳米颗粒@琼脂糖膜的裂解作用及其协同作用在高效催化中的作用

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Thiols are known for stabilizing gold nanoparticles (Au NPs). Herein, an intriguing feasibility of a group of thiols to non-conventionally fragment supported Au NPs in the absence of any auxiliary applied energy is demonstrated. The Au NPs are studded into an agarose hydrogel film as a solid support (Au@Agr), and the group of thiols studied includes thioglycolic acid (TGA), cysteine (CS), 2-mercaptoethanol (ME), L-methionine (MET), thiourea (TU), and 1,3-propanedithiol (PDT). By simply keeping the Au@Agr film immersed into thiol solution for 1 h at room temperature, fragmented nanoparticles of much smaller sizes were obtained. Interestingly, only TGA, CS, ME and MET were found to be capable of successfully fragmenting Au@Agr. A mechanistic interpretation suggests that a prompt transfer of electron density from thiols to Au@Agr can be credited for the fragmentation behaviour of thiols. In addition, the efficacy of such a film in showing an efficient catalytic activity regulated by synergism between thiols and supported Au NPs (Au@Agr) is also presented. TGA and CS fragmented Au@Agr, i.e., TGA-Au@Agr and CS-Au@Agr films, work as an effective catalyst taking similar to 20 to 30 seconds for the complete reduction of p-nitrophenol (p-NP), an industrial pollutant with sluggish removal properties. A pseudo first-order rate for the catalytic p-NP reduction reaction is followed by TGA-Au@Agr as well as CS-Au@Agr with rate constant values determined to be 1.6 x 10(-1) s(-1) and 1.1 x 10(-1) s(-1), respectively. The exclusivity of TGA and CS to swiftly catalyze p-NP reduction and also the individual role of Agr, Au@Agr and TGA/CS-Au@Agr operating in synergy for the successful catalysis was also studied in detail.
机译:已知硫醇可稳定金纳米颗粒(Au NPs)。在本文中,证明了在没有任何辅助施加的能量的情况下,一组硫醇对非常规片段化的负载的Au NPs的吸引人的可行性。金纳米颗粒被钉入琼脂糖水凝胶薄膜中作为固体载体(Au @ Agr),所研究的硫醇包括巯基乙酸(TGA),半胱氨酸(CS),2-巯基乙醇(ME),L-蛋氨酸(MET) ),硫脲(TU)和1,3-丙二酚(PDT)。通过在室温下简单地将Au @ Agr膜浸入硫醇溶液中1 h,就可以得到尺寸更小的碎片纳米颗粒。有趣的是,仅发现TGA,CS,ME和MET能够成功破碎Au @ Agr。机械学解释表明,电子密度从硫醇到Au @ Agr的迅速转移可以归因于硫醇的断裂行为。另外,还提出了这种膜在显示有效的催化活性方面的功效,该活性受硫醇和负载的Au NP(Au @ Agr)之间的协同作用调节。 TGA和CS片段化的Au @ Agr,即TGA-Au @ Agr和CS-Au @ Agr膜,是一种有效的催化剂,完全还原对硝基苯酚(p-NP)所需的时间约为20至30秒。具有缓慢去除性能的工业污染物。催化p-NP还原反应的拟一级反应速率之后是TGA-Au @ Agr和CS-Au @ Agr,其速率常数确定为1.6 x 10(-1)s(-1)和分别为1.1 x 10(-1)s(-1)。还详细研究了TGA和CS快速催化p-NP还原的排他性以及Agr,Au @ Agr和TGA / CS-Au @ Agr在成功催化中协同作用的个别作用。

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