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Shape-selective rhodium nano-huddles on DNA for high efficiency hydrogen evolution reaction in acidic medium
Journal of Materials Chemistry C ( IF 6.4 ) Pub Date : 2020-12-23 , DOI: 10.1039/d0tc05518b
Sangeetha Kumaravel 1, 2, 3, 4, 5 , Kannimuthu Karthick 1, 2, 3, 4, 5 , Selvasundarasekar Sam Sankar 1, 2, 3, 4, 5 , Arun Karmakar 1, 2, 3, 4, 5 , Subrata Kundu 1, 2, 3, 4, 5
Affiliation  

Hydrogen gas (H2) production from electrocatalytic water splitting is one of the main alternative green energy sources to overcome the fossil-based energy demands in future. For large-scale H2 production, properties such as low overpotential, stability, sustainability and resistivity are the major things to address in the designing of an electrocatalyst. In this line, we have constructed a shape-selective ultra-low Rhodium (Rh) nanoparticles (NPs) as an active electrocatalyst for the hydrogen evolution reaction (HER). However, the high cost and scarcity of Rh are barriers to its utilization in large scale electrocatalytic water splitting. The idea of using biomolecule DNA to reduce the Rh metal percentage and also erradicate the use of external binder is an alternate strategy in the field of electrocatalysis. Also, the method of DNA metallization (Rh/DNA) is quite simple to prepare within a short time span of just 15 min in aqueous medium. The resulting DNA mediated Rh nano-huddles (Rh/DNA-1) shows excellent activity in the HER of 0.5 M H2SO4 with a mass loading of 0.007 mg cm−2, which is comparatively 30 times less loading than the commercial loading of 0.205 mg cm−2. Because of this low loading, the observed mass activities were really huge and Rh/DNA-1 showed 1257 A g−1 at an overpotential of 100 mV. Rh/DNA-1 required an overpotential of 105 mV to reach the current density of 10 mA cm−2 and 194 mV for 50 mA cm−2, respectively. Also, it showed excellent stability over 36 000 s at a current density of 10 mA cm−2 in chronoamperometry studies with no loss in activity. Moreover, the catalyst shows a very low charge transfer resistance (Rct) of 1.8 Ω and follows facile kinetics with a lower Tafel value of 68 mV dec−1 for Rh/DNA-1. Further, the TOF was calculated at 300 mV and Rh/DNA-1 showed 0.00064 s−1. For comparison, Rh NPs without DNA were studied for the HER and required 97 mV at 10 mA cm−2 with 0.205 mg cm−2 loading, showing the essentiality of DNA in the electrocatalytic HER study. Therefore, DNA-based electrocatalysts may help to develop cost effective and efficient electrocatalysts in the near future.

中文翻译:

DNA上的形状选择性铑纳米簇可在酸性介质中高效析氢

电催化水分解产生的氢气(H 2)是克服未来化石能源需求的主要替代绿色能源之一。对于大型H 2生产,低电势,稳定性,可持续性和电阻率等特性是电催化剂设计中要解决的主要问题。在这条生产线中,我们构建了形状选择性超低铑(Rh)纳米颗粒(NPs)作为氢析出反应(HER)的活性电催化剂。然而,Rh的高成本和稀缺性阻碍了其在大规模电催化水分解中的利用。在生物催化领域,使用生物分子DNA降低Rh金属含量并消除外部结合剂的使用是一种替代策略。同样,DNA金属化(Rh / DNA)的方法在水性介质中仅15分钟的短时间内即可制备,非常简单。所得的DNA介导的Rh纳米簇(Rh / DNA-1)在HER为0时显示出色的活性。2 SO 4的质量负载为0.007 mg cm -2,比商业负载的0.205 mg cm -2少30倍。由于这种低负荷,观察到的质量活动确实很大,Rh / DNA-1在100 mV的超电势下显示1257 A g -1。Rh / DNA-1需要105 mV的过电势才能分别达到10 mA cm -2的电流密度和194 mV的50 mA cm -2的电流密度。此外,在计时电流分析研究中,在电流密度为10 mA cm -2的情况下,它在36000 s内表现出出色的稳定性,而没有活性损失。此外,该催化剂显示出非常低的电荷转移阻力( R ct)为1.8Ω),并且遵循简单的动力学,Raf / DNA-1的Tafel值较低,为68 mV dec -1。此外,计算出的TOF为300mV,Rh / DNA-1显示为0.00064s -1。为了进行比较,对不含DNA的Rh NPs进行了HER研究,在10 mA cm -2时需要97 mV,负载为0.205 mg cm -2,显示了在电催化HER研究中DNA的重要性。因此,基于DNA的电催化剂可以在不久的将来帮助开发具有成本效益和高效的电催化剂。
更新日期:2021-01-12
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