Ternary Sn‐Ti‐O Electrocatalyst Boosts the Stability and Energy Efficiency of CO<sub>2</sub> Reduction

Wen, Guobin; Ren, Bohua; Park, Moon Gyu; Yang, Jie; Dou, Haozhen; Zhang, Zhen; Deng, Yaping; Bai, Zhengyu; Yang, Lin; Gostick, Jeff T.; Botton, Gianluigi A.; Hu, Yongfeng; Chen, Zhongwei

doi:10.1002/ange.202004149

Cited by 9 publications

(3 citation statements)

References 81 publications

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“…Among electrocatalytic materials studied, Sn is a promising candidate owing to its low cost and planetary abundance 15 , 16 . Sn has strong binding energy for *OCHO, and this favours the first-step CO 2 hydrogenation in CO 2 -to-formate conversion 17 , 18 .…”

Section: Introductionmentioning

confidence: 99%

“…Further improvement of the HCOO – production rate and cathodic energy efficiency (CEE) relative to current benchmarks (Supplementary Table 4 ) requires precise control of the elemental distributions in the active sites. In particular, knowledge of the electrochemical stability of Sn and Sn-based materials in aqueous electrolytes at different pH is lacking; indeed, among reported formate catalysts, it has been challenging to combine optimal adsorption energetics for intermediate binding with sites stable against reconstruction 13 – 16 .…”

Section: Introductionmentioning

confidence: 99%

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Stable, active CO2 reduction to formate via redox-modulated stabilization of active sites

et al. 2021

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Electrochemical reduction of CO2 (CO2R) to formic acid upgrades waste CO2; however, up to now, chemical and structural changes to the electrocatalyst have often led to the deterioration of performance over time. Here, we find that alloying p-block elements with differing electronegativities modulates the redox potential of active sites and stabilizes them throughout extended CO2R operation. Active Sn-Bi/SnO2 surfaces formed in situ on homogeneously alloyed Bi0.1Sn crystals stabilize the CO2R-to-formate pathway over 2400 h (100 days) of continuous operation at a current density of 100 mA cm−2. This performance is accompanied by a Faradaic efficiency of 95% and an overpotential of ~ −0.65 V. Operating experimental studies as well as computational investigations show that the stabilized active sites offer near-optimal binding energy to the key formate intermediate *OCHO. Using a cation-exchange membrane electrode assembly device, we demonstrate the stable production of concentrated HCOO– solution (3.4 molar, 15 wt%) over 100 h.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Stable, active CO2 reduction to formate via redox-modulated stabilization of active sites

et al. 2021

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“…By further analysis, after the bonding of Sn species to CN, N 1 s peaks shift to higher binding energies, clearly indicating the transfer of electrons from N atoms to Sn atoms, which modifies the overall electronic structure of Sn species and the CN substrate [18] . The highly electron‐rich centers of Sn species are presumably favorable for the adsorption/activation of CO 2 and its conversion to intermediates [19] . Meanwhile, the formed electrostatic field would help to promote the charge transport and enhance the electrochemical conversion of CO 2 [8b,13] …”

Section: Resultsmentioning

confidence: 99%

Highly Efficient and Selective CO₂Electro‐Reduction to HCOOH on Sn Particle‐Decorated Polymeric Carbon Nitride

et al. 2020

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Electrochemical conversion of CO 2 into liquid fuels by efficient and earth-abundant catalysts is of broad interest but remains a great challenge in renewable energy production and environmental remediation. Herein, a Sn particle-decorated polymeric carbon nitride (CN) electrocatalyst was successfully developed for efficient, durable, and highly selective CO 2 reduction to formic acid. High-resolution X-ray photoelectron spectroscopy confirmed that the metallic Sn particles and CN matrix are bound by strong chemical interaction, rendering the composite catalyst a stable structure. More notably, the electronic structure of Sn was well tuned to be highly electron-rich due to the electron transfer from N atoms of CN to Sn atoms via metalsupport interactions, which favored the adsorption and activation of CO 2 molecules, promoted charge transport, and thus enhanced the electrochemical conversion of CO 2. The composite electrocatalyst demonstrated an excellent Faradaic efficiency of formic acid (FE HCOOH) up to 96 � 2 % at the potential of À 0.9 V vs. reversible hydrogen electrode, which remained at above 92 % during the electrochemical reaction of 10 h, indicating that the present Sn particle-decorated polymeric carbon nitride electrocatalyst is among the best in comparison with reported Sn-based electrocatalysts.

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In Situ Phase Separation into Coupled Interfaces for Promoting CO₂ Electroreduction to Formate over a Wide Potential Window

Wang

Yang

et al. 2021

Angewandte Chemie

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Bimetallic sulfides are expected to realize efficient CO2 electroreduction into formate over a wide potential window, however, they will undergo in situ structural evolution under the reaction conditions. Therefore, clarifying the structural evolution process, the real active site and the catalytic mechanism is significant. Here, taking Cu2SnS3 as an example, we unveiled that Cu2SnS3 occurred self‐adapted phase separation toward forming the stable SnO2@CuS and SnO2@Cu2O heterojunction during the electrochemical process. Calculations illustrated that the strongly coupled interfaces as real active sites driven the electron self‐flow from Sn4+ to Cu+, thereby promoting the delocalized Sn sites to combine HCOO* with H*. Cu2SnS3 nanosheets achieve over 83.4 % formate selectivity in a wide potential range from −0.6 V to −1.1 V. Our findings provide insight into the structural evolution process and performance‐enhanced origin of ternary sulfides under the CO2 electroreduction.

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Ternary Sn‐Ti‐O Electrocatalyst Boosts the Stability and Energy Efficiency of CO₂ Reduction

Cited by 9 publications

References 81 publications

Stable, active CO2 reduction to formate via redox-modulated stabilization of active sites

Stable, active CO2 reduction to formate via redox-modulated stabilization of active sites

Highly Efficient and Selective CO₂Electro‐Reduction to HCOOH on Sn Particle‐Decorated Polymeric Carbon Nitride

In Situ Phase Separation into Coupled Interfaces for Promoting CO₂ Electroreduction to Formate over a Wide Potential Window

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Ternary Sn‐Ti‐O Electrocatalyst Boosts the Stability and Energy Efficiency of CO2 Reduction

Cited by 9 publications

References 81 publications

Stable, active CO2 reduction to formate via redox-modulated stabilization of active sites

Stable, active CO2 reduction to formate via redox-modulated stabilization of active sites

Highly Efficient and Selective CO2Electro‐Reduction to HCOOH on Sn Particle‐Decorated Polymeric Carbon Nitride

In Situ Phase Separation into Coupled Interfaces for Promoting CO2 Electroreduction to Formate over a Wide Potential Window

Contact Info

Product

Resources

About

Ternary Sn‐Ti‐O Electrocatalyst Boosts the Stability and Energy Efficiency of CO₂ Reduction

Highly Efficient and Selective CO₂Electro‐Reduction to HCOOH on Sn Particle‐Decorated Polymeric Carbon Nitride

In Situ Phase Separation into Coupled Interfaces for Promoting CO₂ Electroreduction to Formate over a Wide Potential Window