<p>As important catalysts for C–C coupling, copper-based materials have great potential for electrocatalytic reduction of CO<sub>2</sub> to C<sub>2+</sub> products. In this work, Cu<sub>2</sub>O catalysts modified with different lanthanide hydroxides were successfully synthesized and used for CO<sub>2</sub> electroreduction. The results showed that compared with Cu<sub>2</sub>O/Gd(OH)<sub>3</sub> and Cu<sub>2</sub>O/Yb(OH)<sub>3</sub> catalysts, Cu<sub>2</sub>O/La(OH)<sub>3</sub> exhibited the highest electrocatalytic performance for CO<sub>2</sub> reduction. This catalyst was able to maintain a high Faraday efficiency for C<sub>2+</sub> products (<InlineEquation ID="IEq1"> <EquationSource Format="TEX">\({\rm FE}_{{\rm C}_{2+}}\)</EquationSource> <EquationSource Format="MATHML"><math display="block"> <msub> <mrow> <mi mathvariant="normal">FE</mi> </mrow> <mrow> <msub> <mrow> <mi mathvariant="normal">C</mi> </mrow> <mrow> <mn>2</mn> <mo>+</mo> </mrow> </msub> </mrow> </msub> </math></EquationSource> </InlineEquation>) of about 60% within the current density range of 400–800 mA cm<sup>−2</sup>. The highest <InlineEquation ID="IEq2"> <EquationSource Format="TEX">\({\rm FE}_{{\rm C}_{2+}}\)</EquationSource> <EquationSource Format="MATHML"><math display="block"> <msub> <mrow> <mi mathvariant="normal">FE</mi> </mrow> <mrow> <msub> <mrow> <mi mathvariant="normal">C</mi> </mrow> <mrow> <mn>2</mn> <mo>+</mo> </mrow> </msub> </mrow> </msub> </math></EquationSource> </InlineEquation> reached 66% at 600 mA cm<sup>−2</sup> and the partial current density for C<sub>2+</sub> products reached a maximum of 488 mA cm<sup>−2</sup>. Meanwhile, the catalyst could run stably for 40 h with a remained <InlineEquation ID="IEq3"> <EquationSource Format="TEX">\({\rm FE}_{{\rm C}_{2+}}\)</EquationSource> <EquationSource Format="MATHML"><math display="block"> <msub> <mrow> <mi mathvariant="normal">FE</mi> </mrow> <mrow> <msub> <mrow> <mi mathvariant="normal">C</mi> </mrow> <mrow> <mn>2</mn> <mo>+</mo> </mrow> </msub> </mrow> </msub> </math></EquationSource> </InlineEquation> of about 60%. Multiple characterizations reveal that the introduction of La(OH)<sub>3</sub> promotes the formation of *CO intermediates, and also helps to stabilize the Cu(I) species in Cu<sub>2</sub>O under cathodic potentials, thus facilitating the C–C coupling for C<sub>2+</sub> production. This work provides a new strategy to enhance the C<sub>2+</sub> production via stabilizing Cu(I).</p>

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Cu2O/lanthanide hydroxide boosting electrocatalytic CO2 reduction via stabilizing Cu(I)

  • Ran Li,
  • Hang Yin,
  • Wen-Kai Jing,
  • Jia-Lin Cheng,
  • Xue-Rong Qin,
  • Tong-Bu Lu,
  • Hong-Juan Wang,
  • Zi-You Yu

摘要

As important catalysts for C–C coupling, copper-based materials have great potential for electrocatalytic reduction of CO2 to C2+ products. In this work, Cu2O catalysts modified with different lanthanide hydroxides were successfully synthesized and used for CO2 electroreduction. The results showed that compared with Cu2O/Gd(OH)3 and Cu2O/Yb(OH)3 catalysts, Cu2O/La(OH)3 exhibited the highest electrocatalytic performance for CO2 reduction. This catalyst was able to maintain a high Faraday efficiency for C2+ products ( \({\rm FE}_{{\rm C}_{2+}}\) FE C 2 + ) of about 60% within the current density range of 400–800 mA cm−2. The highest \({\rm FE}_{{\rm C}_{2+}}\) FE C 2 + reached 66% at 600 mA cm−2 and the partial current density for C2+ products reached a maximum of 488 mA cm−2. Meanwhile, the catalyst could run stably for 40 h with a remained \({\rm FE}_{{\rm C}_{2+}}\) FE C 2 + of about 60%. Multiple characterizations reveal that the introduction of La(OH)3 promotes the formation of *CO intermediates, and also helps to stabilize the Cu(I) species in Cu2O under cathodic potentials, thus facilitating the C–C coupling for C2+ production. This work provides a new strategy to enhance the C2+ production via stabilizing Cu(I).