Improving CO2‐to‐C2 Conversion of Atomic CuFONC Electrocatalysts through F, O‐Codrived Optimization of Local Coordination Environment DOI

Zunhang Lv,

Changli Wang, Yarong Liu

et al.

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(21)

Published: Feb. 27, 2024

Abstract Electrocatalytic CO 2 to multi‐carbon products is an attractive strategy achieve a carbon‐neutral energy cycle. Single‐atom catalysts (SACs) that the C selectivity always have low metal loading and inevitably undergo in situ reversible/irreversible metallic agglomerations under working conditions. Herein, high‐density Cu SA anchored F, O, N co‐doped carbon composites (CuFONC) with stable CuN O 1 configuration provided, which can reach remarkable of ≈80.5% Faradaic efficiency at −1.3 V versus RHE. In situ/ex experimental characterization density functional theory (DFT) calculations verified excellent stability during RR process be attributed F/O co‐derived regulation for CuFONC. Remarkably, as confirmed by DFT, it atomic sites adjacent bonded motifs CuFONC act adsorption * C─C coupling process. This work brings prospective on designing novel but coordination electrolytic ‐to‐C pathway.

Language: Английский

Intermetallic Nanocrystals for Fuel-Cells-Based Electrocatalysis DOI

Fangxu Lin,

Menggang Li, Lingyou Zeng

et al.

Chemical Reviews, Journal Year: 2023, Volume and Issue: 123(22), P. 12507 - 12593

Published: Nov. 1, 2023

Electrocatalysis underpins the renewable electrochemical conversions for sustainability, which further replies on metallic nanocrystals as vital electrocatalysts. Intermetallic have been known to show distinct properties compared their disordered counterparts, and long explored functional improvements. Tremendous progresses made in past few years, with notable trend of more precise engineering down an atomic level investigation transferring into practical membrane electrode assembly (MEA), motivates this timely review. After addressing basic thermodynamic kinetic fundamentals, we discuss classic latest synthetic strategies that enable not only formation intermetallic phase but also rational control other catalysis-determinant structural parameters, such size morphology. We demonstrate emerging nanomaterials potentially advancement energy electrocatalysis. Then, state-of-the-art characterizations representative electrocatalysts emphasis oxygen reduction reaction evaluated a MEA setup. summarize review by laying out existing challenges offering perspective future research directions toward practicing conversions.

Language: Английский

Citations

92
Recent progress on ZIF-8 based MOF derivatives for electrocatalysis DOI

Yuzhuang Song,

Chengzhong Yu, Dingxuan Ma

et al.

Coordination Chemistry Reviews, Journal Year: 2023, Volume and Issue: 499, P. 215492 - 215492

Published: Oct. 27, 2023

Language: Английский

Citations

58
Highly Ordered Hierarchical Porous Single‐Atom Fe Catalyst with Promoted Mass Transfer for Efficient Electroreduction of CO2 DOI Creative Commons
Chen Jia, Yong Zhao, Shuang Song

et al.

Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 13(37)

Published: Aug. 10, 2023

Abstract Electrocatalysts are crucial to drive the electrochemical carbon dioxide reduction reaction (CO 2 RR) which lower energy barrier, tune intricate pathways and suppress competitive side‐reaction. Beyond efficient active sites advantageous local environment, a rapid mass transfer ability is also for catalyst design. However, it rare that research has been done investigate in detail process CO RR, expose underlying relationship between final performance. Here, single‐atom Fe‐N‐C shown with highly ordered porous substrate containing hierarchical micropores, mesopores, macropores. Such delicate structure significantly facilitates toward isolated Fe sites, achieving excellent RR performance, especially limited region H‐cell maximum partial current density of ‐19 mA cm −2 . Operando impedance spectroscopy relevant distributed relaxation times analysis reveal rapidly decreased resistance increase potential. The Lattice Boltzmann method Discrete Element (LBM‐DEM) simulations further performed exhibit origin enhanced performance from facilitated gas diffusion process.

Language: Английский

Citations

53
Photocoupled Electroreduction of CO2 over Photosensitizer-Decorated Covalent Organic Frameworks DOI

Qiu‐Jin Wu,

Duan‐Hui Si,

Shihua Ye

et al.

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(36), P. 19856 - 19865

Published: Aug. 31, 2023

Introducing an external visible-light field would be a promising strategy to improve the activity of electrocatalytic CO2 reduction reaction (CO2RR), but it still remains challenge due short excited-state lifetime active sites. Herein, Ru(bpy)3Cl2 struts as powerful photosensitive donors were immobilized into backbones Co-porphyrin-based covalent organic frameworks (named Co-Bpy-COF-Rux, x is molar ratio Ru and Co species, = 1/2 2/3) via coordination bonds, for photo-coupled CO2RR produce CO. The optimal Co-Bpy-COF-Ru1/2 displays high CO Faradaic efficiency 96.7% at -0.7 V vs reversible hydrogen electrode (RHE) partial current density 16.27 mA cm-2 -1.1 RHE under assistance light, both which far surpassing values observed in dark. significantly enhanced mainly attributed incorporation donor with long concomitantly giant built-in electric Co-Bpy-COF-Ru1/2, efficiently accelerate photo-induced electron transfer from cobalt-porphyrin light. Thus, sites have longer lower rate-determining steps' energy occurring during actual process. This first work porphyrin-based COFs CO2RR, opening new frontier construction efficient electrocatalysts.

Language: Английский

Citations

52
Recent progress of MOF-functionalized nanocomposites: From structure to properties DOI
Kun Xu, Songtao Zhang,

Xiaoli Zhuang

et al.

Advances in Colloid and Interface Science, Journal Year: 2023, Volume and Issue: 323, P. 103050 - 103050

Published: Nov. 10, 2023

Language: Английский

Citations

51
Engineering organic polymers as emerging sustainable materials for powerful electrocatalysts DOI
Xun Cui, Mingjie Wu,

Xueqin Liu

et al.

Chemical Society Reviews, Journal Year: 2024, Volume and Issue: 53(3), P. 1447 - 1494

Published: Jan. 1, 2024

A comprehensive overview on organic polymers as electrocatalysts is summarized. By presenting the engineering strategies, insightful understandings, challenges, and perspectives, we hope this review can provide valuable references for readers.

Language: Английский

Citations

41
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

33
Lignin‐Metal Supramolecular Framework Strategy of Self‐Healing Carbon‐Coated CoRu Alloy Nanocatalyst for Efficient Overall Water Splitting DOI
Xuliang Lin,

Dalang Chen,

Xueqing Qiu

et al.

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(32)

Published: June 19, 2024

Abstract Common precursors for carbon materials typically include petroleum‐based polymers or MOF materials. However, these often encounter challenges such as metal aggregation, high cost, and metals leaching. In this work, a novel of approach lignin‐metal supramolecular framework complex (MSF@Lignin) is introduced. These complexes are formed through oxidative ammonolysis lignin (OAL) to synthesize nitrogen‐doped carbon‐encapsulated CoRu nanocatalyst (CoRu@OALC) via in situ carbonization. CoRu@OALC exhibited exceptional performance both HER (90 mV) OER (200 at the current density 10 mA cm −2 , with an overall water splitting voltage 1.5 V outstanding stability under density. During pyrolysis process, became encapsulated by lignin‐derived carbon, occurring within temperature range 600–700 °C. catalytic active sites primarily located defects showcasing unique “self‐healing” phenomenon layer. Oxygen‐containing intermediates ( * OH, O, OOH) facilitated reconstruction on layer, while hydrogen‐containing H) contributed reappearance defect‐rich structure.

Language: Английский

Citations

32
Covalent Organic Frameworks as Promising Platforms for Efficient Electrochemical Reduction of Carbon Dioxide: A Review DOI Creative Commons
Zihao Chen, Nan Li, Qichun Zhang

et al.

Small Structures, Journal Year: 2024, Volume and Issue: 5(5)

Published: Feb. 5, 2024

In current research, achieving carbon neutrality has become a primary focus through the utilization of various conversion technologies that transform dioxide (CO 2 ) into valuable chemicals or fuels. Covalent organic frameworks (COFs), as emerging crystalline polymers, offer distinct advantages in CO compared to other materials. These include controllable nanoscale pores, predefined functional units, editable framework structures, and rich conjugated systems. The unique characteristics COFs make them highly promising electrocatalysts for conversion. This review provides comprehensive overview pioneering works recent research on COF‐based materials electrochemical reduction reaction. offers analysis design principles reactive sites, skeleton pore functionalities, 3D frameworks, morphologies, composite COFs, aiming enhance electrocatalysis. Finally, this presents some recommendations material design, reaction mechanisms, theoretical computations understanding mechanisms further facilitate high‐performance electrocatalysts.

Language: Английский

Citations

31
Ionic Covalent Organic Frameworks in Adsorption and Catalysis DOI
Minghao Liu, Qing Xu, Gaofeng Zeng

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(22)

Published: April 2, 2024

The ion extraction and electro/photo catalysis are promising methods to address environmental energy issues. Covalent organic frameworks (COFs) a class of template construct absorbents catalysts because their stable frameworks, high surface areas, controllable pore environments, well-defined catalytic sites. Among them, ionic COFs as unique crystalline porous materials, with charges in the or along walls, have shown different properties resulting performance these applications those from charge-neutral COFs. In this review, current research progress based on for conversion, including cationic/anionic materials is reviewed terms synthesis strategy, modification methods, mechanisms adsorption catalysis, well applications. Finally, we demonstrated challenges future development design strategies

Language: Английский

Citations

31