Selective electrocatalytic reduction of carbon dioxide to oxalate by lead tin oxides with low overpotential

Cheng, Yingying; Hou, Pengfei; Pan, Hui; Shi, Han; Kang, Peng

doi:10.1016/j.apcatb.2020.118954

Cited by 46 publications

(54 citation statements)

References 42 publications

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“…Furthermore, the Pb 4f 5/2 was also observed at the binding energy at 143.06 eV corresponding to the Pb(II) oxidation state such as Pb 3 (CO 3 ) 2 (OH) 2 (Cheng et al, 2020).…”

Section: Mineral Precipitationmentioning

confidence: 97%

Mechanistic Insight of Biochar-layered Double Hydroxide Composite for Efficient Removal of Aqueous Pb(II) and Cu(II)

Chen

et al. 2021

Preprint

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To explore the heavy metal adsorption mechanisms by biochar-based materials, MgAl-layered double hydroxide (MgAl-LDH) was loaded on a commercial coconut shell biochar (BC) to obtain the composite (BC-LDH) for adsorptive decontamination of Pb(II) and Cu(II) in water. The removal capacities of BC-LDH (294 and 38.6 mg/g) was higher than BC (13.3 and 11.4 mg/g) and LDH (126 and 22.7 mg/g) for aqueous Pb(II) and Cu(II). The pseudo-second-order equation and the Langmuir model could better illustrate the adsorption process, respectively. The interaction mechanisms between BC-LDH and heavy metals were classified as mineral precipitation (Qpre), cation exchange and isomorphic replacement (Qexc), electrostatic attraction (Qele), and surface complexation (Qcom) according to the characterization results. The quantitative analysis indicated that the contributions of the above mechanisms of BC-LDH for Pb(II) and Cu(II) followed the order of Qpre > Qele > Qexc and Qpre > Qexc > Qele, respectively. Compared with BC, the Qpre increased and Qele decreased significantly, certified the combination of BC and LDH provided a kind of viable composite in heavy metal wastewater treatment.

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“…Furthermore, the Pb 4f 5/2 was also observed at the binding energy at 143.06 eV corresponding to the Pb(II) oxidation state such as Pb 3 (CO 3 ) 2 (OH) 2 (Cheng et al, 2020).…”

Section: Mineral Precipitationmentioning

confidence: 97%

Mechanistic Insight of Biochar-layered Double Hydroxide Composite for Efficient Removal of Aqueous Pb(II) and Cu(II)

Chen

et al. 2021

Preprint

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“…1 This work reported a carbon enrichment strategy using surface immobilized amines for integrated CO 2 capture and conversion in f lue gas electroreduction. • Bi, J.; Hou, P.; Liu, F. W.; Kang 4 This study reported a synergistic ef fect between Pb and Sn in binary lead tin oxide to lower the overpotential for oxalate formation.…”

Section: ■ Key Referencesmentioning

confidence: 99%

“…33 We employed a binary lead tin oxide, PbSnO 3 /C, catalyst, which could efficiently catalyze CO 2 electroreduction to oxalate at low overpotentials in 0.1 M tetra-n-butylammonium hexafluorophosphate in propylene carbonate (0.1 M nBu 4 NPF 6 /PC), and maximum oxalate FE of 85.1% was achieved. 4 The synergy between Pb and Sn is critical for the high efficiency, and neither of lead oxide or tin oxide catalysts could achieve the high FE or small overpotential. In PbSnO 3 /C, the surface Pb ions were initially reduced to Pb 0 to form Pb 0 −SnO x structure.…”

Section: Nanostructured Catalystsmentioning

confidence: 99%

CO₂ Electrolysis System under Industrially Relevant Conditions

Cheng

Hou

Wang³

et al. 2022

Acc. Chem. Res.

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Conspectus Carbon dioxide emissions from consumption of fossil fuels have caused serious climate issues. Rapid deployment of new energies makes renewable energy driven CO2 electroreduction to chemical feedstocks and carbon-neutral fuels a feasible and cost-effective pathway for achieving net-zero emission. With the urgency of the net-zero goal, we initiated our research on CO2 electrolysis with emphasis on industrial relevance. The CO2 molecules are thermodynamically stable due to high activation energy of the two CO bonds, and efficient electrocatalysts are required to overcome the sluggish dynamics and competitive hydrogen evolution reaction. The CO2 electrocatalysts that we have explored include molecular catalysts and nanostructured catalysts. Molecular catalysts are centered on earth abundant elements such as Fe and Co for catalyzing CO2 reduction, and using Fe catalysts, we proposed an amidation strategy for reduction of CO2 to methanol, bypassing the inactive formate pathway. For nanostructured catalysts, we developed a carbon enrichment strategy using nitrogen-rich nanomaterials for selective CO2 reduction. Direct CO2 electroreduction from the flue gas stream represents the “holy grail” in the field, because typical CO2 concentration in flue gas is only 6–15%, posing a significant challenge for CO2 electrolysis. On the other hand, direct electroreduction of CO2 in the flue gas eliminates the carbon capture process and simplifies the overall carbon capture and utilization (CCU) scheme. However, direct flue gas reduction is frustrated by the reactive oxygen (5–8%), low CO2 concentration (6–15%), and potentially toxic impurities. Surface CO2 enrichment catalysts with high O2 tolerance could be viable for achieving direct CO2 electroreduction for decarbonization of flue gas. In addition to the electrocatalysts, the incorporation of catalysts into the electrolyzer and development of a suitable process was also investigated to meet industrial demands. A membrane electrode assembly (MEA) is a zero-gap configuration with cathode and anode catalysts coated on either side of an ion exchange membrane. We adopted the MEA configuration due to the structural simplicity, low ohmic resistance, and high efficiency. The electrode factors (for example, membrane type, catalyst layer porosity, and MEA fabrication method) and the electrolyzer factors (for example, flow channels, gas diffusion layer) are critical to highly efficient operation. We separately developed an anion-exchange membrane-based system for CO production and cation-exchange membrane-based system for formate production. The optimized electrolyzer configuration can generate uniform current and voltage distribution in a large-area electrolyzer and operate using an industrial CO2 stream. The optimized process was developed with the targets of long-term continuous operation and no electrolyte consumption.

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“…[9,25] The electrochemically active surface area (ECSA) of the above catalysts were evaluated by the electrochemical double-layer capacitance (C dl ) (Figure S6, Supporting Information). [26] The C dl value of CuSn(OH) 6 (0.09 mF cm À 2 ) was higher than Cu(OH) 2 (0.04 mF cm À 2 ), CuSn(OH) x -41 (0.05 mF cm À 2 ), CuSn(OH) x -11 (0.04 mF cm À 2 ), CuSn(OH) x -12 (0.03 mF cm À 2 ) and Sn(OH) x (0.07 mF cm À 2 ), indicating that the increased surface area was beneficial to the dAOR performance.…”

Section: Daor Mechanismmentioning

confidence: 99%

CuSn Double‐Metal Hydroxides for Direct Electrochemical Ammonia Oxidation to Dinitrogen

et al. 2022

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Direct electrochemical ammonia oxidation reaction (dAOR) to form N2 is of great significance to process ammonia‐containing wastewater or to make efficient ammonia fuel cells. Herein, CuSn double‐metal hydroxides are synthesized via a co‐precipitation method and used in dAOR with 10 mM normalNnormalH3 −N Among the synthesized hydroxides, CuSn(OH)6 shows a decent N2 −N partial current density (1.2 mA cm−2) and a substantially higher N2 −N Faradaic efficiency (84.5 %). In situ infrared spectroscopy confirms that the intermediacy of normalN2normalHnormaly dimeric species facilitates the formation of desired N2 product during the dAOR process. The synergy between Cu and Sn is critical for the enhanced dAOR activity, as Cu serves as the catalytic center while Sn adsorbs normalNnormalH3 −N intensively.

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Selective electrocatalytic reduction of carbon dioxide to oxalate by lead tin oxides with low overpotential

Cited by 46 publications

References 42 publications

Mechanistic Insight of Biochar-layered Double Hydroxide Composite for Efficient Removal of Aqueous Pb(II) and Cu(II)

Mechanistic Insight of Biochar-layered Double Hydroxide Composite for Efficient Removal of Aqueous Pb(II) and Cu(II)

CO₂ Electrolysis System under Industrially Relevant Conditions

CuSn Double‐Metal Hydroxides for Direct Electrochemical Ammonia Oxidation to Dinitrogen

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Selective electrocatalytic reduction of carbon dioxide to oxalate by lead tin oxides with low overpotential

Cited by 46 publications

References 42 publications

Mechanistic Insight of Biochar-layered Double Hydroxide Composite for Efficient Removal of Aqueous Pb(II) and Cu(II)

Mechanistic Insight of Biochar-layered Double Hydroxide Composite for Efficient Removal of Aqueous Pb(II) and Cu(II)

CO2 Electrolysis System under Industrially Relevant Conditions

CuSn Double‐Metal Hydroxides for Direct Electrochemical Ammonia Oxidation to Dinitrogen

Contact Info

Product

Resources

About

CO₂ Electrolysis System under Industrially Relevant Conditions