Heterogeneous Cobalt Phthalocyanine/Sulfur‐Modified Hollow Carbon Sphere for Boosting CO2 Electroreduction and Zn–CO2 Batteries
Authors:
- 27 December 2023
- journal article
- research article
- Published by Wiley in Advanced Functional Materials
- Vol. 34 (14)
Abstract
Tuning coordination environment of single‐atom catalysts (SACs) is widely applied for the electrochemical CO2 reduction reaction (CO2RR). However, the influence of the interaction between SACs and support on the catalytic performance are not comprehensive. Herein, taking cobalt phthalocyanine (CoPc) as a conceptual example, a hetero S‐atom doping strategy of hollow carbon sphere (S‐NHC) is put forward as a carrier, revealing the intrinsic relationship between microenvironment regulation and catalytic activity of single Co‐atom. The additional S doping may induce more carbon defect and increases the content of pyrrolic N in the S‐NHC sample, leading to stronger electronic interaction of heterogeneous CoPc/S‐NHC for boosting CO2RR performance. Remarkably, the catalyst achieves a highest CO selectivity of nearly 100% at −0.6 V, and the FECO are over 90% in a wide potential range from −0.4 to −0.8 V in a flow cell. The maximum power density is high as 2.68 mW cm−2 at 4.7 mA cm−2 for the Zn–CO2 battery with CoPc/S‐NHC cathode. In situ attenuated total reflection infrared (ATR‐IR) spectroscopy reveals the formation of key *COOH and *CO intermediates, while the calculation result confirm the optimized Gibbs free energy of these intermediates on CoPc/S‐NHC, suggesting the feasibility of the regulation strategy.Keywords
Funding Information
- National Natural Science Foundation of China (22205205)
This publication has 46 references indexed in Scilit:
- Catalytic Mechanisms and Design Principles for Single‐Atom Catalysts in Highly Efficient CO2 ConversionAdvanced Energy Materials, 2019
- Aqueous CO2 Reduction with High Efficiency Using α‐Co(OH)2‐Supported Atomic Ir ElectrocatalystsAngewandte Chemie International Edition, 2019
- Steric Modification of a Cobalt Phthalocyanine/Graphene Catalyst To Give Enhanced and Stable Electrochemical CO2 Reduction to COACS Energy Letters, 2019
- Existence of an Electrochemically Inert CO Population on Cu Electrodes in Alkaline pHACS Catalysis, 2018
- Homogeneously Dispersed Co9S8 Anchored on Nitrogen and Sulfur Co-Doped Carbon Derived from Soybean as Bifunctional Oxygen Electrocatalysts and SupercapacitorsACS Applied Materials & Interfaces, 2018
- Design of Single-Atom Co–N5 Catalytic Site: A Robust Electrocatalyst for CO2 Reduction with Nearly 100% CO Selectivity and Remarkable StabilityJournal of the American Chemical Society, 2018
- Co Nanoparticles/Co, N, S Tri-doped Graphene Templated from In-Situ-Formed Co, S Co-doped g-C3N4 as an Active Bifunctional Electrocatalyst for Overall Water SplittingACS Applied Materials & Interfaces, 2017
- Highly selective and active CO2 reduction electrocatalysts based on cobalt phthalocyanine/carbon nanotube hybrid structuresNature Communications, 2017
- Nanostructured Materials for Heterogeneous Electrocatalytic CO2 Reduction and their Related Reaction MechanismsAngewandte Chemie International Edition, 2017
- High Catalytic Activity of Nitrogen and Sulfur Co‐Doped Nanoporous Graphene in the Hydrogen Evolution ReactionAngewandte Chemie International Edition, 2014