Selectivity-Enhanced Electroreduction of CO2 to CO at Novel Ru-Linked-GO Nanohybrids: the Role of Nanoarchitecture DOI
Neda Khedri, Ali Reza Mahjoub, Amir Hossein Cheshme Khavar

et al.

Inorganic Chemistry, Journal Year: 2024, Volume and Issue: 63(17), P. 7571 - 7588

Published: April 18, 2024

Recently, global-scale efforts have been conducted for the electroreduction of CO2 as a potentially beneficial pathway conversion greenhouse gases to useful chemicals and renewable fuels. This study focuses on development selective sustainable electrocatalysts reduction aqueous CO. A RuIIcomplex [Ru(tptz)(ACN)Cl2] (RCMP) (tptz = 2,4,6-tris(2-pyridyl)-1,3,5-triazine, ACN acetonitrile) was prepared molecular electrocatalyst reaction in an solution. Density functional theory-calculated frontier orbitals suggested that tptz ligand plays key role dictating electrocatalytic reactions. The RCMP grafted onto graphene oxide (GO) surface both noncovalently (GO/RCMP) covalently (GO-RCMP). field emission scanning electron microscopy elemental distribution analyses revealed homogeneous complex GO sheet. photoluminescence spectra confirmed accelerated charge-transfer nanohybrids. Compared bare complex, GO-RCMP GO/RCMP nanohybrids showed enhanced activity, achieving >95% 90% Faradaic efficiencies CO production at more positive onset potentials, respectively. nanohybrid demonstrated outstanding activity with current ∼84 μA. offers perspective outer- inner-sphere electron-transfer mechanisms electrochemical energy systems.

Language: Английский

Electronic Structure Design of Transition Metal-Based Catalysts for Electrochemical Carbon Dioxide Reduction DOI Creative Commons
Liang Guo, Jingwen Zhou, Fu Liu

et al.

ACS Nano, Journal Year: 2024, Volume and Issue: 18(14), P. 9823 - 9851

Published: March 28, 2024

With the increasingly serious greenhouse effect, electrochemical carbon dioxide reduction reaction (CO2RR) has garnered widespread attention as it is capable of leveraging renewable energy to convert CO2 into value-added chemicals and fuels. However, performance CO2RR can hardly meet expectations because diverse intermediates complicated processes, necessitating exploitation highly efficient catalysts. In recent years, with advanced characterization technologies theoretical simulations, exploration catalytic mechanisms gradually deepened electronic structure catalysts their interactions intermediates, which serve a bridge facilitate deeper comprehension structure-performance relationships. Transition metal-based (TMCs), extensively applied in CO2RR, demonstrate substantial potential for further modulation, given abundance d electrons. Herein, we discuss representative feasible strategies modulate catalysts, including doping, vacancy, alloying, heterostructure, strain, phase engineering. These approaches profoundly alter inherent properties TMCs interaction thereby greatly affecting rate pathway CO2RR. It believed that rational design modulation fundamentally provide viable directions development toward conversion many other small molecules.

Language: Английский

Citations

43
Coordination Environment Engineering of Metal Centers in Coordination Polymers for Selective Carbon Dioxide Electroreduction toward Multicarbon Products DOI
Juan Wang, Mingzi Sun, Hongming Xu

et al.

ACS Nano, Journal Year: 2024, Volume and Issue: 18(9), P. 7192 - 7203

Published: Feb. 22, 2024

Electrocatalytic carbon dioxide reduction reaction (CO2RR) toward value-added chemicals/fuels has offered a sustainable strategy to achieve carbon-neutral energy cycle. However, it remains great challenge controllably and precisely regulate the coordination environment of active sites in catalysts for efficient generation targeted products, especially multicarbon (C2+) products. Herein we report engineering metal centers polymers electroreduction CO2 C2+ products under neutral conditions. Significantly, Cu polymer with Cu–N2S2 configuration (Cu–N–S) demonstrates superior Faradaic efficiencies 61.2% 82.2% ethylene respectively, compared selective formic acid on an analogous Cu–I2S2 mode (Cu–I–S). In situ studies reveal balanced formation atop bridge *CO intermediates Cu–N–S, promoting C–C coupling production. Theoretical calculations suggest that can induce electronic modulations sites, where d-band center is upshifted Cu–N–S stronger selectivity Consequently, displays trend while Cu–I–S favors due suppression couplings pathways large barriers.

Language: Английский

Citations

33
Site‐selective Growth of fcc‐2H‐fcc Copper on Unconventional Phase Metal Nanomaterials for Highly Efficient Tandem CO2 Electroreduction DOI Creative Commons
Yangbo Ma, Mingzi Sun, Hongming Xu

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(32)

Published: May 29, 2024

Abstract Copper (Cu) nanomaterials are a unique kind of electrocatalysts for high‐value multi‐carbon production in carbon dioxide reduction reaction (CO 2 RR), which holds enormous potential attaining neutrality. However, phase engineering Cu remains challenging, especially the construction unconventional Cu‐based asymmetric heteronanostructures. Here site‐selective growth on unusual gold (Au) nanorods, obtaining three kinds heterophase fcc‐2H‐fcc Au–Cu heteronanostructures is reported. Significantly, resultant Janus nanostructures (JNSs) break symmetric mode Au. In electrocatalytic CO RR, JNSs exhibit excellent performance both H‐type and flow cells, with Faradaic efficiencies 55.5% 84.3% ethylene products, respectively. situ characterizations theoretical calculations reveal co‐exposure 2H‐Au 2H‐Cu domains diversifies CO* adsorption configurations promotes spillover subsequent C–C coupling toward generation reduced energy barriers.

Language: Английский

Citations

18
Steering the Selectivity of Carbon Dioxide Electroreduction from Single-Carbon to Multicarbon Products on Metal–Organic Frameworks via Facet Engineering DOI
Pengyi Lu,

Jia Lv,

Yu Chen

et al.

Nano Letters, Journal Year: 2024, Volume and Issue: 24(5), P. 1553 - 1562

Published: Jan. 24, 2024

Although metal-organic frameworks (MOFs) have attracted more attention for the electrocatalytic CO

Language: Английский

Citations

15
High entropy alloy electrocatalysts DOI

Guoliang Gao,

Yangyang Yu, Guang Zhu

et al.

Journal of Energy Chemistry, Journal Year: 2024, Volume and Issue: 99, P. 335 - 364

Published: Aug. 3, 2024

Language: Английский

Citations

14
Electrochemical CO2 Reduction: Advances, Insights, Challenges, and Future Directions DOI Creative Commons
Asghar Ali, Muhammad Qasim, S. Sakhi

et al.

Materials Today Sustainability, Journal Year: 2025, Volume and Issue: unknown, P. 101089 - 101089

Published: Feb. 1, 2025

Language: Английский

Citations

2
Green, efficient and controllable synthesis of high-quality MOF-74 with high gravity technology DOI

Xinran Shi,

Meng Qiao,

Yan Wei

et al.

Green Chemistry, Journal Year: 2024, Volume and Issue: 26(10), P. 6209 - 6218

Published: Jan. 1, 2024

A green, efficient high-gravity-assisted approach was proposed to synthesize MOF-74–Co with controllable particle size, high crystallinity, large specific surface area and excellent CO 2 adsorption performance.

Language: Английский

Citations

8
Room temperature synthesized layered CAU-17 MOFs for highly active and selective electrocatalytic CO2 reduction to formate DOI

Linhua Mi,

Bin Chen,

Xin Xu

et al.

Journal of Alloys and Compounds, Journal Year: 2024, Volume and Issue: 978, P. 173516 - 173516

Published: Jan. 13, 2024

Language: Английский

Citations

6
Confined CuⅠ sites in partially electro-reduced 2D conductive Cu-MOF film for boosting CO2 electrocatalysis to C2 products DOI
Bing Chang,

Fengtao Zhang,

Zhaojun Min

et al.

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 496, P. 153993 - 153993

Published: July 14, 2024

Language: Английский

Citations

6
Electronic Structure Modulation of Unconventional Phase Metal Nanomaterials for Highly Selective Carbon Dioxide Electroreduction DOI
Juan Wang, Haoyi Tan, Hongming Xu

et al.

ACS Materials Letters, Journal Year: 2023, Volume and Issue: 5(12), P. 3212 - 3221

Published: Nov. 6, 2023

The electrochemical carbon dioxide (CO2) reduction reaction (CO2RR) has been considered as a promising approach to convert atmospheric CO2 value-added chemicals promote neutrality. However, developing electrocatalysts with superior activity and high selectivity toward individual products remains great challenge. Herein we report the electronic structure modulation of unconventional phase metal nanomaterials achieve highly efficient electroreduction. It found that growing cerium oxide (CeOx) nanostructures on 4H/face-centered cubic (fcc) gold (Au) nanorods can significantly enhance their catalytic conversion monoxide. X-ray analysis indicates change 4H/fcc Au after CeOx overgrowth. In-situ attenuated total reflection infrared spectroscopy measurements reveal HCO3– concentration near surface Au-CeOx heteronanostructures is much higher than nanorods, facilitating process. Density functional theory calculations suggest activation effect nanorod for electrocatalytic CO2RR. synergy between promotes formation carboxyl (*COOH) species thus boosts CO2RR performance. This work highlights importance rational regulation unusual small molecules.

Language: Английский

Citations

13