Selective electroreduction of CO2 to formate by a heterogenized Ir complex using H2O as an electron/hydrogen source†

EES catalysis Pub Date : 2024-12-06 DOI:10.1039/D4EY00261J

Jieun Jung, Keun Woo Lee, Naonari Sakamoto, Selvam Kaliyamoorthy, Taku Wakabayashi, Kenji Kamada, Keita Sekizawa, Shunsuke Sato, Tomiko M. Suzuki, Takeshi Morikawa and Susumu Saito

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Abstract

A newly synthesized tetradentate PNNP-coordinated iridium (Ir) complex, Mes-IrPPh2, immobilized on a carbon material, was found to be a superior catalyst for CO₂ electrochemical reduction reaction (CO₂ERR) to give formate, (HCOO⁻), allowing an operation near the theoretical potential (−0.18 V vs. RHE, pH = 7.3) in water. The combined [Mes-IrPPh2] electrode furnished HCOO⁻ with a current density of greater than 2.2 to 7.7 mA cm⁻² over −0.27 to −0.47 V vs. RHE, providing faradaic efficiencies (FE) of >90%. The outstanding robustness of the electrode attained continuous production of HCOO⁻ up to 12.5 mmol with 2.86 μmol of Mes-IrPPh2 at −0.27 V vs. RHE over 168 h. Furthermore, solar-driven electrochemical CO₂ reduction to HCOO⁻ was also carried out in water with a Ni/Fe–Ni foam anode as a water oxidation catalyst and a silicon photovoltaic cell to achieve a solar-to-formate conversion efficiency (η_STF) of 13.7%.

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利用H2O作为电子/氢源†，用多相Ir络合物选择性电还原CO2生成甲酸

新合成的四价pnnp配位铱（Ir）配合物Mes-IrPPh2固定在碳材料上，是CO2电化学还原反应（CO2ERR）生成甲酸（HCOO -）的优越催化剂，可在水中接近理论电位（- 0.18 V vs. RHE, pH = 7.3）进行操作。复合[Mes-IrPPh2]电极为HCOO−提供了大于2.2至7.7 mA cm−2的电流密度，比RHE在−0.27至−0.47 V之间，法拉第效率（FE）为>；90%。该电极的鲁棒性使其在- 0.27 V与RHE条件下，以2.86 μmol的Mes-IrPPh2在168h内连续生成12.5 mmol的HCOO−。此外，在Ni/ Fe-Ni泡沫阳极作为水氧化催化剂和硅光伏电池的条件下，太阳能驱动CO2电化学还原为HCOO−，太阳能-甲酸转化效率（ηSTF）达到13.7%。

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EES catalysis

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