Formic acid dehydrogenation over PdNi alloys supported on N-doped carbon: synergistic effect of Pd–Ni alloying on hydrogen release

Literature Information

Publication Date 2021-04-30
DOI 10.1039/D1CP00236H
Impact Factor 3.676
Authors

Rizcky Tamarany, Dong Yun Shin, Sukho Kang, Hyangsoo Jeong, Jun Kim, Dong-Hee Lim


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Abstract

Bimetallic Pd1Nix alloys supported on nitrogen-doped carbon (Pd1Nix/N–C, x = 0.37, 1.3 and 3.6) exhibit higher activities than Pd/N–C towards dehydrogenation of formic acid (HCO2H, FA). Density functional theory (DFT) calculations provided electronic and atomic structures, energetics and reaction pathways on Pd(111) and Pd1Nix(111) surfaces of different Pd/Ni compositions. A density of states (DOS) analysis disclosed the electronic interactions between Pd and Ni revealing novel active sites for FA dehydrogenation. Theoretical analysis of FA dehydrogenation on Pd1Nix(111) (x = 0.33, 1 and 3) shows that the Pd1Ni1(111) surface provides optimum H2-release efficiency via a favorable ‘HCOO pathway’, in which a hydrogen atom and one of the two oxygen atoms of FA interact directly with surface Ni atoms producing adsorbed CO2 and H2. The enhanced efficiency is also attributed to the blocking of an unfavorable ‘COOH pathway’ through which a C–O bond is broken and side products of CO and H2O are generated.

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Source Journal

Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics
CiteScore: 5.5
Self-citation Rate: 10.3%
Articles per Year: 3036

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.

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