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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2021 · IF 8.128

Bifunctional effect of Bi(OH)3 on the PdBi surface as interfacial Brønsted base enables ethanol electro-oxidization

Jialu Huang,Chengwei Deng,Yue Liu,Tingting Han,Feng Ji,Yuehua Zhang,Hongbin Lu,Ping Hua,Bowei Zhang,Tao Qian,Xiaolei Yuan,Yaoyue Yang,Yong Yao

Palladium (Pd) is supposed to be one of the most promising catalytic metals towards ethanol (C 2 H 5 OH) oxidation reaction (EOR). However, Pd electrocatalysts easily suffer from the poisoning of the intermediates (especially CO), resulting in the quick decay of EOR catalysis. Herein, inspired by the Brønsted-Lowry acid-base theory, a “attraction–repulsion” concept is proposed to guide the surface structure engineering toward EOR catalysts. Specifically, we induce Bi(OH) 3 species as Brønsted base onto PdBi nanoplates to effectively repel the adsorption of CO intermediates. The PdBi-Bi(OH) 3 nanoplates show an impressive mass activity of 4.46 A mg Pd -1 during the EOR catalysis and keep excellent stability. Both the stability and enhanced performance are attributed by the interfacial Brønsted base Bi(OH) 3 which can selectively attract and repel reactants and intermediates, as evidenced from in situ measurements and theoretical views.

研究领域: 材料科学 · 电化学 · 催化作用
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GREEN CHEMISTRY · 2021 ·Vol. 23 ·期 21 ·8571-8580 · IF 10.182

Insight into the reversible behavior of Lewis–Brønsted basic poly(ionic liquid)s in one-pot two-step chemical fixation of CO2 to linear carbonates

Yuting He,Huimin Lu,Xue Li,Jun Wu,Tiancheng Pu,Wei Du,Hongping Li,Jing Ding,Hui Wan,Guofeng Guan

The multi-step reaction of CO2 over basic catalysts significantly improves the diversity of products, vividly embodying the ability of green chemistry to turn waste into treasure. However, under a Lewis acidic CO2 atmosphere, the activity maintenance of the multi-step reaction puts forward higher requirements for the reversible regeneration ability of the basic catalysts. Novel Lewis–Brønsted binary basic poly(ionic liquid)s (LB-PILs) were successfully developed through a radical copolymerization followed by ion-exchange strategy, and were applied to the two-step synthesis of dimethyl carbonate (DMC) by coupling CO2 cycloaddition and CH3OH transesterification without any cocatalyst. Relying on the activation of CO2 by Lewis basic tertiary N and the thermal recovery of nucleophilic HCO3− to stronger Brønsted basic OH− with the help of temperature control in CH3OH transesterification, the LB-PILs presented high activity, stable repeatability and linear carbonate universality. In situ IR analysis and Knoevenagel condensation, combined with theoretical calculations, provided reliable support for the ingenious incorporation of reversible regeneration of basic catalysts in a Lewis acidic CO2 atmosphere and multi-step coupling reaction process of CO2.

研究领域: 化学工程 · 绿色化学 · 催化材料
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Inorganic and Nano-Metal Chemistry · 2021 · IF 1.716

Syntheses and structural characterization of eight inorganic-organic hybrid solids based on N-Brønsted bases and halometallates of Zn, Cu, Sb and Bi

Jiahua Guo,Yuqi Zhang,Shouwen Jin,Xiaoyun Ye,Kaikai Hu,Weiqiang Xu,Daqi Wang

Eight organic-inorganic hybrid salts [(HL1)(SbCl4)] (1) (L1 = N,N-dimethylbenzylamine), [(HL2)2(ZnCl4)] (2) (L2 = 4-chlorobenzylamine), [(HL2)(L2)(CuCl3)(H2O)2] (3), [(HL3)2(Sb2OCl6)] (4) (L3 = quinoline), [(HL4)4(Bi2Cl10)] (5) (L4 = 2-methylquinoline), [(HL5)(SbCl4)] (6) (L5 = 5,7-dimethyl-1,8-naphthyridine-2-amine), [(H2L6)(SbCl5)] (7) (L6 = 3,6-bis(imidazol-1-yl)pyridazine) and [(H2L7)2(CuBr4)2] · 7H2O (8) (L7 = di(2-benzimidazol-1-ylethyl)ether) were prepared and characterized by IR, XRD, EA and TG analysis. XRD analysis told that all of the complexes were 3 D net built from non-covalent bonds from the cations and the halometallates. The aryl rings of the cations in all of the compounds are essentially planar. The H2O also had crucial role in structure extension in 3 and 8. Extensive intermolecular interactions have been used in the self-assembly of diverse motifs, ranging from strong N-H···X (X = Br, Cl), N-H···O, N-H···N, O-H···O, O-H···Br H-bonds to weak CH2···O, CH3-Cl/CH2-Cl/CH-Cl, Cl-Cl, O-Br, CH3-π, CH2-π, Cl-π and π-π associations. The arrangements of the anions and cations in the solid are ruled not only by the size and symmetry of the cations, but also by the non-covalent bonds in the crystal structures.

研究领域: 无机化学 · 材料科学
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