<p>The electrocatalytic reduction of carbon dioxide reaction (CO<sub>2</sub>RR) to multi-carbon (C<sub>2+</sub>) products attracts substantial attention due to its profound research implications and commercial value in chemical manufacturing. However, the competitive hydrogen evolution reaction (HER) and sluggish C–C coupling procedure pose significant impediments to the selectivity of C<sub>2+</sub> products under industrial current density. Herein, we report an interfacial nanoconfinement strategy with <i>N</i>-(2-acetamido)iminodiacetic acid (ADA) to engineer a series of capping layer-covered Cu (Cu@ADA-x) catalysts, showing a characteristic volcano-type correlation between gradient-distributed capping thickness and C<sub>2+</sub> products selectively. Consequently, Cu@ADA-m reaches maximum Faradaic efficiency of C<sub>2+</sub> <InlineEquation ID="IEq1"> <EquationSource Format="TEX">\((\text{FE}_{\mathrm{C}_{2+}})\)</EquationSource> <EquationSource Format="MATHML"><math display="block"> <mo stretchy="false">(</mo> <msub> <mtext>FE</mtext> <mrow> <msub> <mrow> <mi mathvariant="normal">C</mi> </mrow> <mrow> <mn>2</mn> <mo>+</mo> </mrow> </msub> </mrow> </msub> <mo stretchy="false">)</mo> </math></EquationSource> </InlineEquation> of 86.8% and exceptional durability, maintaining over 80% of initial <InlineEquation ID="IEq2"> <EquationSource Format="TEX">\(\text{FE}_{\mathrm{C}_{2+}}\)</EquationSource> <EquationSource Format="MATHML"><math display="block"> <msub> <mtext>FE</mtext> <mrow> <msub> <mrow> <mi mathvariant="normal">C</mi> </mrow> <mrow> <mn>2</mn> <mo>+</mo> </mrow> </msub> </mrow> </msub> </math></EquationSource> </InlineEquation> after 42 h at 200 mA cm<sup>−2</sup>, along with an energy efficiency of C<sub>2+</sub> products of 38.5%. <i>In-situ</i> Raman spectroscopy and density functional theory (DFT) calculations demonstrated that in addition to stabilizing the metastable catalytic Cu species, the confinement of capping architecture creates optimal gas adsorption capacity, thus promoting the utilization efficiency of crucial *CO intermediate and lowering the energy barriers for the C–C coupling step. This work redefines catalyst design principles for carbon-neutral electrochemical manufacturing of multi-carbon products at an industrial scale.</p>

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Efficient CO2 electroreduction to multi-carbon products by nanoconfinement strategy over Cu catalyst at industrial current density

  • Ye Bai,
  • Hong Liu,
  • Xin Wang,
  • Tixuan Xia,
  • Yingchen Yang,
  • Jinhao Chen,
  • Jinhui Hao,
  • Cai Ning,
  • Weidong Shi

摘要

The electrocatalytic reduction of carbon dioxide reaction (CO2RR) to multi-carbon (C2+) products attracts substantial attention due to its profound research implications and commercial value in chemical manufacturing. However, the competitive hydrogen evolution reaction (HER) and sluggish C–C coupling procedure pose significant impediments to the selectivity of C2+ products under industrial current density. Herein, we report an interfacial nanoconfinement strategy with N-(2-acetamido)iminodiacetic acid (ADA) to engineer a series of capping layer-covered Cu (Cu@ADA-x) catalysts, showing a characteristic volcano-type correlation between gradient-distributed capping thickness and C2+ products selectively. Consequently, Cu@ADA-m reaches maximum Faradaic efficiency of C2+ \((\text{FE}_{\mathrm{C}_{2+}})\) ( FE C 2 + ) of 86.8% and exceptional durability, maintaining over 80% of initial \(\text{FE}_{\mathrm{C}_{2+}}\) FE C 2 + after 42 h at 200 mA cm−2, along with an energy efficiency of C2+ products of 38.5%. In-situ Raman spectroscopy and density functional theory (DFT) calculations demonstrated that in addition to stabilizing the metastable catalytic Cu species, the confinement of capping architecture creates optimal gas adsorption capacity, thus promoting the utilization efficiency of crucial *CO intermediate and lowering the energy barriers for the C–C coupling step. This work redefines catalyst design principles for carbon-neutral electrochemical manufacturing of multi-carbon products at an industrial scale.