Construction of efficient Pb(ii) carboxylate catalysts for the oxygen and hydrogen evolution reactions†

IF 3.5 3区 化学 Q2 CHEMISTRY, INORGANIC & NUCLEAR
Janak, Vijay S. Sapner, Bhaskar R. Sathe and Sadhika Khullar
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Abstract

The development of cost-effective and efficient electrocatalysts can solve the problems associated with the production of energy via water-splitting reactions. In this work, we have focused on two lead-based coordination polymers (CPs), namely, {[Pb2(TPBN)(HBTC)2]2·2.5H2O}n (CP1) and {[Pb2(TPBN)(NDC)2]·H2O}n (CP2), that were synthesized by self-assembly method at room temperature in good yields. The two-dimensional structures of CP1 and CP2 were determined by single-crystal X-ray diffraction studies. Their phase purity and thermal stability were confirmed by powder X-ray diffraction and TGA analysis, respectively. In addition to this, Hirshfeld surface analysis of CP1 and CP2 revealed the key differences in their intermolecular interactions. Both CP1 and CP2 were employed for HER and OER. It has been found that the change in the carboxylate from BTC to NDC resulted in better electrocatalytic activity towards water-splitting reactions. This may be attributed to the presence of more π character in NDC compared to BTC, which makes the electron flow much easier for HER process. CP1 and CP2 showed overpotential values of −0.58 V and −0.55 V, respectively, in 1 M H2SO4 to reach a 10 mA cm−2 current density with Tafel slopes of 31 mV dec−1 and 25 mV dec−1, respectively. For the OER process, CP1 and CP2 exhibited overpotentials of 590 mV and 470 mV, respectively, in 1 M KOH at a current density of 50 mA cm−2 with Tafel slope values of 81 mV dec−1 and 56 mV dec−1, respectively. Turnover frequency (TOF) values of CP1 and CP2 were 1.05 s−1 and 3.21 s−1 for OER and 1.97 s−1 and 9.65 s−1 for HER, respectively. These results indicate that both CPs can act as highly efficient electrocatalysts for clean energy production.

Abstract Image

构建用于氧和氢进化反应的高效羧酸铅(II)催化剂
开发具有成本效益的高效电催化剂可以解决通过水分离反应生产能源的问题。在这项工作中,我们重点研究了两种铅基配位聚合物(CPs){[Pb2(TPBN)(HBTC)2]2⸱5H2O}n(CP1)和{[Pb2(TPBN)(NDC)2].H2O}n(CP2),这两种聚合物是通过自组装方法在室温下合成的,产率良好。单晶 X 射线衍射测定了 CP1 和 CP2 的二维结构。它们的相纯度和热稳定性分别通过粉末衍射和 TGA 分析得到了再次确认。此外,对 CP1 和 CP2 进行的 Hirshfeld 表面分析也显示了这两种氯化石蜡分子间相互作用的关键差异。CP1 和 CP2 均用于 HER 和 OER。研究发现,将羧基从 BTC 改为 NDC 后,水分离反应的电催化活性更好。这可能是因为与 BTC 相比,NDC 中存在更多 π 特性,从而使电子流更容易进入 HER 过程。在 1 M H2SO4 中,CP1 和 CP2 的过电位值分别为 580 mV 和 550 mV,电流密度为 10 mA cm-2,塔菲尔斜率分别为 31 mV dec-1 和 25 mV dec-1。在 OER 过程中,CP1 和 CP2 在 1 M KOH 中的过电位分别为 590 mV 和 470 mV,电流密度为 50 mA cm-2,塔菲尔斜率值分别为 56 mV dec-1 和 81 mV dec-1。CP1 和 CP2 的翻转频率(TOF)在 OER 中分别为 1.05 s-1 和 3.21 s-1,在 HER 中分别为 1.97 s-1 和 9.65 s-1。
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来源期刊
Dalton Transactions
Dalton Transactions 化学-无机化学与核化学
CiteScore
6.60
自引率
7.50%
发文量
1832
审稿时长
1.5 months
期刊介绍: Dalton Transactions is a journal for all areas of inorganic chemistry, which encompasses the organometallic, bioinorganic and materials chemistry of the elements, with applications including synthesis, catalysis, energy conversion/storage, electrical devices and medicine. Dalton Transactions welcomes high-quality, original submissions in all of these areas and more, where the advancement of knowledge in inorganic chemistry is significant.
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