This work presents that Cu with atomic-scale spacings ( d s ) efficiently catalyses the electrochemical co-reduction of CO 2 and NO 3 − to urea. Specifically, Cu with d s near 6 Å (6 Å-Cu) produces urea with a high yield rate and partial current density.
Immobilizing Low‐Cost Metal Nitrides in Electrochemically Reconstructed Platinum Group Metal (PGM)‐Free Oxy‐(Hydroxides) Surface for Exceptional OER Kinetics in Anion Exchange Membrane Water Electrolysis (Adv. Energy Mater. 6/2023)
Oxygen Evolution Reaction In article number 2203401, Youngkook Kwon, and co-workers demonstrate an energy-efficient, low-cost oxygen-evolving electrode by immobilizing Ni3N particles on an electrochemically reconstructed V-NiFeOOH surface for sustainable water oxidation in anion exchange membrane water electrolyzers.
Interface rich CuO/Al<sub>2</sub>CuO<sub>4</sub> surface for selective ethylene production from electrochemical CO<sub>2</sub> conversion
Siraj Sultan, Hojeong Lee, Sojung Park, Minho M. Kim, Aram Yoon, Hansaem Choi, Tae‐Hoon Kong, Young-Jin Koe, Hyung‐Suk Oh, Zonghoon Lee, Hyungjun Kim, Wooyul Kim, Youngkook Kwon
IF 30.8
Energy & Environmental Science
In this work, we designed a novel CuO/Al 2 CuO 4 catalyst by a phase and interphase engineering approach, which enables the electrochemical conversion of carbon dioxide to ethylene with ultrahigh activity and selectivity.
Immobilizing Low‐Cost Metal Nitrides in Electrochemically Reconstructed Platinum Group Metal (PGM)‐Free Oxy‐(Hydroxides) Surface for Exceptional OER Kinetics in Anion Exchange Membrane Water Electrolysis
Abstract A highly efficient and platinum group metal (PGM)‐free oxygen evolution reaction (OER) electrode is developed by immobilizing Ni 3 N particles on the electrochemically reconstructed amorphous oxy‐hydroxides surface, resulting in a twofold higher industrial relevance current density of 1 A cm geo −2 at an ultra‐small overpotential η( O 2 ) of 271 mV, with a high turnover frequency of 2.53 s −1 , high Faradic efficiency of 99.6 % and exceptional OER stability of 1000 h in continuous electrolysis. Such a unique amorphous‐crystalline interface with enriched active sites greatly facilitates electron transport and OER kinetics at the electrode‐electrolyte interface. Further, combined with an efficient PGM‐free cathode (MoNi 4 /MoO 2 @Ni), this electrode demonstrates a current density of 685 mA cm geo −2 at 1.85 V cell at 70 °C in an anion exchange membrane water electrolyzer (AEMWE) operated with ultra‐pure water‐electrolyte. These findings highlight the design of highly‐efficient oxygen‐evolving catalysts and significant advancement in the practical implementation of AEMWEs for grid‐scale hydrogen production.
Atomic‐Scale Spacing between Copper Facets for the Electrochemical Reduction of Carbon Dioxide
Hyung Mo Jeong, Youngkook Kwon, Jong Ho Won, Yanwei Lum, Mu‐Jeng Cheng, Kwang Ho Kim, Martin Head‐Gordon, Jeung Ku Kang
IF 26
Advanced Energy Materials
Abstract Copper (Cu) offers a means for producing value‐added fuels through the electrochemical reduction of carbon dioxide (CO 2 ), i.e., the CO 2 reduction reaction (CO 2 RR), but designing Cu catalysts with significant Faradaic efficiency to C 2+ products remains as a great challenge. This work demonstrates that the high activity and selectivity of Cu to C 2+ products can be achieved by atomic‐scale spacings between two facets of Cu particles. These spacings are created by lithiating CuO x particles, removing lithium oxides formed, and electrochemically reducing CuO x to metallic Cu. Also, the range of spacing ( d s ) is confirmed via the 3D tomographs using the Cs‐corrected scanning transmission electron microscopy (3D tomo‐STEM), and the operando X‐ray absorption spectra show that oxidized Cu reduces to the metallic state during the CO 2 RR. Moreover, control of d s to 5–6 Å allows a current density exceeding that of unmodified CuO x nanoparticles by about 12 folds and a Faradaic efficiency of ≈80% to C 2+ . Density functional theory calculations support that d s of 5–6 Å maximizes the binding energies of CO 2 reduction intermediates and promotes C–C coupling reactions. Consequently, this study suggests that control of d s can be used to realize the high activity and C 2+ product selectivity for the CO 2 RR.
This work presents that Cu with atomic-scale spacings ( d s ) efficiently catalyses the electrochemical co-reduction of CO 2 and NO 3 − to urea. Specifically, Cu with d s near 6 Å (6 Å-Cu) produces urea with a high yield rate and partial current density.
Immobilizing Low‐Cost Metal Nitrides in Electrochemically Reconstructed Platinum Group Metal (PGM)‐Free Oxy‐(Hydroxides) Surface for Exceptional OER Kinetics in Anion Exchange Membrane Water Electrolysis (Adv. Energy Mater. 6/2023)
Oxygen Evolution Reaction In article number 2203401, Youngkook Kwon, and co-workers demonstrate an energy-efficient, low-cost oxygen-evolving electrode by immobilizing Ni3N particles on an electrochemically reconstructed V-NiFeOOH surface for sustainable water oxidation in anion exchange membrane water electrolyzers.
Interface rich CuO/Al<sub>2</sub>CuO<sub>4</sub> surface for selective ethylene production from electrochemical CO<sub>2</sub> conversion
Siraj Sultan, Hojeong Lee, Sojung Park, Minho M. Kim, Aram Yoon, Hansaem Choi, Tae‐Hoon Kong, Young-Jin Koe, Hyung‐Suk Oh, Zonghoon Lee, Hyungjun Kim, Wooyul Kim, Youngkook Kwon
IF 30.8
Energy & Environmental Science
In this work, we designed a novel CuO/Al 2 CuO 4 catalyst by a phase and interphase engineering approach, which enables the electrochemical conversion of carbon dioxide to ethylene with ultrahigh activity and selectivity.
Immobilizing Low‐Cost Metal Nitrides in Electrochemically Reconstructed Platinum Group Metal (PGM)‐Free Oxy‐(Hydroxides) Surface for Exceptional OER Kinetics in Anion Exchange Membrane Water Electrolysis
Abstract A highly efficient and platinum group metal (PGM)‐free oxygen evolution reaction (OER) electrode is developed by immobilizing Ni 3 N particles on the electrochemically reconstructed amorphous oxy‐hydroxides surface, resulting in a twofold higher industrial relevance current density of 1 A cm geo −2 at an ultra‐small overpotential η( O 2 ) of 271 mV, with a high turnover frequency of 2.53 s −1 , high Faradic efficiency of 99.6 % and exceptional OER stability of 1000 h in continuous electrolysis. Such a unique amorphous‐crystalline interface with enriched active sites greatly facilitates electron transport and OER kinetics at the electrode‐electrolyte interface. Further, combined with an efficient PGM‐free cathode (MoNi 4 /MoO 2 @Ni), this electrode demonstrates a current density of 685 mA cm geo −2 at 1.85 V cell at 70 °C in an anion exchange membrane water electrolyzer (AEMWE) operated with ultra‐pure water‐electrolyte. These findings highlight the design of highly‐efficient oxygen‐evolving catalysts and significant advancement in the practical implementation of AEMWEs for grid‐scale hydrogen production.
Atomic‐Scale Spacing between Copper Facets for the Electrochemical Reduction of Carbon Dioxide
Hyung Mo Jeong, Youngkook Kwon, Jong Ho Won, Yanwei Lum, Mu‐Jeng Cheng, Kwang Ho Kim, Martin Head‐Gordon, Jeung Ku Kang
IF 26
Advanced Energy Materials
Abstract Copper (Cu) offers a means for producing value‐added fuels through the electrochemical reduction of carbon dioxide (CO 2 ), i.e., the CO 2 reduction reaction (CO 2 RR), but designing Cu catalysts with significant Faradaic efficiency to C 2+ products remains as a great challenge. This work demonstrates that the high activity and selectivity of Cu to C 2+ products can be achieved by atomic‐scale spacings between two facets of Cu particles. These spacings are created by lithiating CuO x particles, removing lithium oxides formed, and electrochemically reducing CuO x to metallic Cu. Also, the range of spacing ( d s ) is confirmed via the 3D tomographs using the Cs‐corrected scanning transmission electron microscopy (3D tomo‐STEM), and the operando X‐ray absorption spectra show that oxidized Cu reduces to the metallic state during the CO 2 RR. Moreover, control of d s to 5–6 Å allows a current density exceeding that of unmodified CuO x nanoparticles by about 12 folds and a Faradaic efficiency of ≈80% to C 2+ . Density functional theory calculations support that d s of 5–6 Å maximizes the binding energies of CO 2 reduction intermediates and promotes C–C coupling reactions. Consequently, this study suggests that control of d s can be used to realize the high activity and C 2+ product selectivity for the CO 2 RR.
A Structure‐Defined Cu(I) Dual‐Atom Catalyst with a Cu <sub>2</sub> N <sub>6</sub> Motif in a Metal‐Organic Framework for CO Electroreduction
Jonghoon Park, Namgyoo Park, Wei‐Sen Chen, Sojung Park, Sujee Cho, Eunji Jin, Jae Hwa Lee, Wooyul Kim, Wonyoung Choe, Mu‐Jeng Cheng, Youngkook Kwon, Hoi Ri Moon
Angewandte Chemie
Abstract The electroreduction of carbon monoxide (CO) provides a sustainable pathway to valuable multi‐carbon (C 2+ ) products, contributing to carbon neutrality. Enhancing coupling efficiency and selectivity for C 2+ formation hinges on precise control of the spatial arrangement of catalytic sites where CO molecules adsorb. Here, we introduce a structurally well‐defined Cu(I) dual‐atom catalyst (DAC) embedded in a metal‐organic framework (MOF) that is synthesized via a thermal transformation. Single‐crystal X‐ray diffraction (SCD) reveals Cu 2 N 6 motifs with a Cu–Cu distance of 3.6 Å, stabilized by tetrazolate within a 2D layer, ensuring CO accessibility and efficient coupling. The catalyst achieves a Faradaic efficiency (FE) of 72% for C 2+ products at a partial current density of −430 mA cm −2 , and a maximum C 2+ FE of 86% at a total current density of −200 mA cm −2 . In situ spectroscopy and density functional theory (DFT) calculations reveal that the paired Cu nodes stabilize key C 2 intermediates via distinct binding configurations, underpinning the system's exceptional performance.
Integration of biomass valorization and bicarbonate electrolysis for low-voltage production of value-added chemicals
Dohee Kim, Hyeonuk Choi, Hojeong Lee, Eunui An, Yoonyoung Kim, Youngkook Kwon, Jihun Oh
IF 8.7
Applied Surface Science Advances
Bicarbonate electrolysis (BCE) utilizing captured CO 2 holds promise for the production of carbon-based chemicals and fuels but exhibits a low energy efficiency due to the high theoretical voltage required to drive the anodic oxygen evolution reaction (OER). Herein, BCE is coupled with the glycerol electrochemical oxidation reaction (GEOR) instead of the OER to decrease the operation voltage and obtain glycolic acid (GCA) and other valuable products. The mechanism of the GEOR, which is catalyzed by a gold nanoparticles embedded nickel oxides combined with multi-walled carbon nanotube (Au-NiO-CNT), is probed by examining the effects of electrolyte alkalinity, with further insights provided by in situ Raman and electrochemical impedance spectroscopic analyses. The incorporated carbon nanotubes increase the catalyst's conductivity, promoting the formation of α-Ni(OH) 2 on the NiO support during the GEOR and thus facilitating the establishment of Ni–OH moieties and their reaction with the primary hydroxyl groups of glycerol to increase GCA selectivity at low applied potentials. Compared with OER-coupled BCE, our process features an ∼890 mV lower operation voltage at 150 mA cm –2 , high CO (86.7 % in 3 M KHCO 3 ) and GCA (25.5 % in 0.1 M glycerol and 3 M KOH) selectivities, and a 16 % lower energy consumption at 150 mA cm –2 (76.76 vs. 91.38 MWh per ton CO).
Energy‐Efficient Dual Formate Electrosynthesis via Coupled Formaldehyde Oxidation and CO <sub>2</sub> Reduction at Ultra‐Low Cell Voltage
Hyoseok Kim, Wonsik Jang, Jin Ho Lee, Hojeong Lee, Seunghyun Lee, Jongkyoung Kim, Dongrak Oh, Woo Yeong Noh, Miri Kim, Sun Gwan, Jongchan Kim, Jae Sung Lee, Youngkook Kwon, Seungho Cho
Angewandte Chemie
Abstract Electrochemical formate (HCOO − ) production via CO 2 reduction reaction (CO 2 RR) holds great promise for carbon‐neutral energy systems; however, its practical implementation is significantly hindered by the high energy demand of anodic oxygen evolution reaction (OER). Replacing OER with a more energetically and economically favorable alternative anodic reaction is therefore essential. In this study, we developed a highly efficient Cu–Ag catalyst for anodic formaldehyde oxidation reaction (FOR). Systematic investigations employing in situ Raman spectroscopy and comprehensive electrochemical analyses revealed that Cu enables an earlier onset potential for FOR, and Ag enhances formaldehyde adsorption, leading to synergistically improved performance. The optimal Cu 3 Ag 7 catalyst exhibited superior FOR performance, with an onset potential of −0.05 V versus the reversible hydrogen electrode ( V RHE ) and Faradaic efficiencies for HCOO − exceeding 90% from 0.1 to 0.5 V RHE . When coupled with CO 2 RR, the FOR||CO 2 RR system enabled dual‐side HCOO − production, achieving a total HCOO − yield rate of 0.39 mmol h −1 cm −2 at an ultra‐low cell voltage of 0.5 V, surpassing the performance of previously reported electrochemical HCOO − production systems. Furthermore, this study presents a versatile anodic strategy that integrates FOR with a range of cathodic reactions, offering an energy‐efficient chemical synthesis approach for the advancement of sustainable electrochemical technologies.
A Structure‐Defined Cu(I) Dual‐Atom Catalyst with a Cu <sub>2</sub> N <sub>6</sub> Motif in a Metal‐Organic Framework for CO Electroreduction
Jonghoon Park, Namgyoo Park, Wei-Sen Chen, Sojung Park, Sujee Cho, Eunji Jin, Jae Hwa Lee, Wooyul Kim, Wonyoung Choe, Mu‐Jeng Cheng, Youngkook Kwon, Hoi Ri Moon
IF 16.9
Angewandte Chemie International Edition
The electroreduction of carbon monoxide (CO) provides a sustainable pathway to valuable multi-carbon (C<sub>2+</sub>) products, contributing to carbon neutrality. Enhancing coupling efficiency and selectivity for C<sub>2+</sub> formation hinges on precise control of the spatial arrangement of catalytic sites where CO molecules adsorb. Here, we introduce a structurally well-defined Cu(I) dual-atom catalyst (DAC) embedded in a metal-organic framework (MOF) that is synthesized via a thermal transformation. Single-crystal X-ray diffraction (SCD) reveals Cu<sub>2</sub>N<sub>6</sub> motifs with a Cu-Cu distance of 3.6 Å, stabilized by tetrazolate within a 2D layer, ensuring CO accessibility and efficient coupling. The catalyst achieves a Faradaic efficiency (FE) of 72% for C<sub>2+</sub> products at a partial current density of -430 mA cm<sup>-2</sup>, and a maximum C<sub>2+</sub> FE of 86% at a total current density of -200 mA cm<sup>-2</sup>. In situ spectroscopy and density functional theory (DFT) calculations reveal that the paired Cu nodes stabilize key C<sub>2</sub> intermediates via distinct binding configurations, underpinning the system's exceptional performance.