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<p>The development of efficient catalysts for CO<sub>2</sub> hydrogenation to formic acid is a key challenge in sustainable chemistry, offering promising pathways for carbon utilization and renewable energy storage. In this study, a series of PdCu<sub>x</sub>/C catalysts were prepared and systematically evaluated under optimized reaction conditions. Among them, PdCu<sub>0.5</sub>/C demonstrated superior activity by achieving a TON of 3732 for formic acid in a dimethylformamide, water and triethylamine solution with excellent stability over multiple cycles. Detailed characterizations confirmed that introducing an optimized amount of Cu effectively reduced the particle size of Pd to 2.6&#xa0;nm, improved metal dispersion and promoted the reduction of Pd<sup>2+</sup> to Pd<sup>0</sup>. The presence of Cu not only induced strong electronic interactions with Pd, enhancing Pd’s electron density and hydrogen dissociation ability, but also facilitated CO<sub>2</sub> activation through increased CO<sub>2</sub> adsorption and hydrogen spillover to adjacent Cu sites. These synergistic effects led to the formation of well-alloyed Pd–Cu bimetallic nanoparticles with superior catalytic properties that stem from a reduced reaction activation energy (Ea = 17.33&#xa0;kJ&#xa0;mol<sup>−1</sup>). The kinetically calculated reaction orders in equation <InlineEquation ID="IEq1"> <EquationSource Format="TEX">\(R = k \cdot P_{{{\text{CO}}_{2} }}^{0.29} \cdot P_{{{\text{H}}_{2} }}^{0.24}\)</EquationSource> <EquationSource Format="MATHML"><math> <mrow> <mi>R</mi> <mo>=</mo> <mi>k</mi> <mo>·</mo> <msubsup> <mi>P</mi> <mrow> <msub> <mtext>CO</mtext> <mn>2</mn> </msub> </mrow> <mrow> <mn>0.29</mn> </mrow> </msubsup> <mo>·</mo> <msubsup> <mi>P</mi> <mrow> <msub> <mtext>H</mtext> <mn>2</mn> </msub> </mrow> <mrow> <mn>0.24</mn> </mrow> </msubsup> </mrow> </math></EquationSource> </InlineEquation> for PdCu<sub>0.5</sub>/C indicate that both reactants were activated more efficiently over Pd–Cu alloys relative to monometallic Pd/C. Overall, the pivotal role of Cu in tuning both the structure and the reaction pathway highlights PdCu<sub>0.5</sub>/C as an efficient and stable catalyst for sustainable CO<sub>2</sub> hydrogenation to formic acid.</p>

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Catalytic hydrogenation of CO2 to formic acid over Cu-promoted Pd nano-alloys supported on carbon

  • 期刊论文

  • 发表日期：

    2026年4月25日

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  • Faisal Irshad,
  • Hamzah A. S. M. Yaseen,
  • Dan Zhang,
  • Xianming Zhu,
  • Shengping Wang

摘要

The development of efficient catalysts for CO2 hydrogenation to formic acid is a key challenge in sustainable chemistry, offering promising pathways for carbon utilization and renewable energy storage. In this study, a series of PdCux/C catalysts were prepared and systematically evaluated under optimized reaction conditions. Among them, PdCu0.5/C demonstrated superior activity by achieving a TON of 3732 for formic acid in a dimethylformamide, water and triethylamine solution with excellent stability over multiple cycles. Detailed characterizations confirmed that introducing an optimized amount of Cu effectively reduced the particle size of Pd to 2.6 nm, improved metal dispersion and promoted the reduction of Pd2+ to Pd0. The presence of Cu not only induced strong electronic interactions with Pd, enhancing Pd’s electron density and hydrogen dissociation ability, but also facilitated CO2 activation through increased CO2 adsorption and hydrogen spillover to adjacent Cu sites. These synergistic effects led to the formation of well-alloyed Pd–Cu bimetallic nanoparticles with superior catalytic properties that stem from a reduced reaction activation energy (Ea = 17.33 kJ mol−1). The kinetically calculated reaction orders in equation \(R = k \cdot P_{{{\text{CO}}_{2} }}^{0.29} \cdot P_{{{\text{H}}_{2} }}^{0.24}\) R = k · P CO 2 0.29 · P H 2 0.24 for PdCu0.5/C indicate that both reactants were activated more efficiently over Pd–Cu alloys relative to monometallic Pd/C. Overall, the pivotal role of Cu in tuning both the structure and the reaction pathway highlights PdCu0.5/C as an efficient and stable catalyst for sustainable CO2 hydrogenation to formic acid.