Palladium (II) pyridylidene sulfonamides (PYSAs) for electrocatalytic reduction of CO2

IF 4 2区化学 Q2 CHEMISTRY, PHYSICAL

Journal of Molecular Structure Pub Date : 2024-11-13 DOI:10.1016/j.molstruc.2024.140582

Afshan Khurshid , Muhammad Nawaz Tahir , Tilo Söhnel , Ehsan Ullah Mughal , Ryan J. Trovitch , M. Naveed Zafar

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Abstract

A new class of donor flexible nitrogen ligands, namely pyridylidene sulfonamides (PYSAs; N-(1-benzylpyridin-4(1H)-ylidene)benzene-sulfonamide, N-(1-benzylpyridin-4(1H)-ylidene)thiophene-2-sulfonamide, N-(1-benzylpyridin-4(1H)-ylidene)pyridine-2-sulfonamide and N-(1-benzylpyridin-4(1H)-ylidene)-8-quinoline-sulfonamide), were prepared from 4-amino-1-benzylpyridin-1-ium chloride and various aromatic sulfonyl chlorides. The treatment of PYSAs with [(CH₃CN)₂PdCl₂] afforded the corresponding Pd(II) complexes. The newly synthesized compounds were characterized by multinuclear ¹H and ¹³C NMR spectroscopy, IR spectroscopy, elemental analysis, and single-crystal X-ray diffraction. Their redox chemistry was then evaluated under an inert atmosphere of nitrogen and carbon dioxide, both in the presence and absence of protons. An apparent interaction of CO₂ with each Pd(II) catalyst was inferred by the collection of cyclic voltammograms and the enhancement of peak currents at respective peak potentials. All catalysts were robust under bulk electrolysis conditions over 3600 s.

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用于电催化还原二氧化碳的钯 (II) 亚吡啶磺酰胺 (PYSA)

一类新的供体柔性氮配体，即吡啶亚磺酰胺（PYSAs）；N-(1-苄基吡啶-4(1H)-亚基)苯磺酰胺、N-(1-苄基吡啶-4(1H)-亚基)噻吩-2-磺酰胺、N-(1-苄基吡啶-4(1H)-亚基)噻吩-2-磺酰胺、N-(1-苄基吡啶-4(1H)-亚基)吡啶-2-磺酰胺和 N-(1-苄基吡啶-4(1H)-亚基)-8-喹啉-磺酰胺）由 4-氨基-1-苄基吡啶-1-鎓氯化物和各种芳香族磺酰氯制备而成。用[(CH3CN)2PdCl2]处理PYSAs，可得到相应的钯(II)配合物。新合成的化合物通过多核 1H 和 13C NMR 光谱、红外光谱、元素分析和单晶 X 射线衍射进行了表征。然后，在氮气和二氧化碳的惰性气氛下，在质子存在和不存在的情况下，对它们的氧化还原化学性质进行了评估。通过收集循环伏安图和峰值电位下峰值电流的增强，可以推断出二氧化碳与每种钯（II）催化剂之间存在明显的相互作用。在 3600 秒的批量电解条件下，所有催化剂都很稳定。

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来源期刊

Journal of Molecular Structure 化学-物理化学

CiteScore

7.10

自引率

15.80%

发文量

2384

审稿时长

45 days

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