Spin Regulation of Nickel Single Atom Catalyst via Axial Phosphor‐Coordination Achieves Near Unity CO Selectivity in Electrochemical CO2 Reduction DOI

Kanghua Miao,

Jundi Qin,

Siyuan Lai

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 26, 2024

Abstract The engineering of the spin state and axial coordination metal center single‐atom catalyst (SAC) represents an effective strategy for regulating catalytic activity, selectivity, stability toward electrocatalytic reduction CO 2 (ECO R). However, rational design deliberate fabrication SACs with specified atoms remain challenging. Herein, Ni single phosphorus (NiP−N 4 −C) four planar nitrogen are fabricated, which induces reorientation 3d orbitals atom shift from low (S = 0) to high 2). enhanced d−p orbital coupling between adsorbents enhances activation reduces energy barrier formation * COOH, a key intermediate in ECO R produce CO, enabling activity near unity selectivity broad potential range 600 mV (−0.4–−1.0 V vs reversible hydrogen electrode RHE), achieving turnover frequency 37.2 s −1 at −1.0 versus RHE. As bifunctional cathode electrocatalyst, NiP−N −C demonstrates peak power density 18.5 mW cm −2 maintains cycling durability over 70 h rechargeable Zn−CO batteries.

Language: Английский

Synergistic Catalysis of Cobalt Single Atoms and Clusters Loaded on Carbon Film: Enhancing Peroxymonosulfate Activation for Degradation of Norfloxacin DOI

Chenglin Hao,

Tinghang Li,

Yanjie Xie

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 1, 2024

Abstract Many existing research focuses on the differences or performance comparisons between single‐atom small‐sized nanocluster catalysts, but there is a lack of comprehensive coupling relationship structure and activity mechanism synergy. This study investigates combined catalytic potential cobalt single atoms (SAs) nanoclusters (NCs) for enhanced peroxymonosulfate (PMS) activation to degrade norfloxacin (NFX). A novel Co SAs‐NCs /CN/TiO 2 catalyst synthesized, featuring SAs NCs uniformly dispersed carbon film wrapping TiO , degradation efficiency NFX solution almost completely degraded, with mineralization rate 76.35%. Density functional theory (DFT) calculations indicate that synergistic interaction promotes more efficient PMS adsorption significantly reduces energy barrier, which enhances electron transfer increases reactive oxygen species (ROS) generation. highlights robust versatile nature this system in addressing various contaminants. elucidates providing new ideas advanced oxidation processes (AOPs) environmental remediation, linking emphasizes practicality importance effectively long‐term remediation water pollutants.

Language: Английский

Citations

16
Enhanced Local CO Coverage on Cu Quantum Dots for Boosting Electrocatalytic CO2 Reduction to Ethylene DOI
Yan Wang, Jiarui Wang, Rui Cai

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 29, 2024

Abstract Ethylene (C 2 H 4 ) electrosynthesis from the electrocatalytic CO reduction process holds enormous potential applications in industrial production. However, sluggish kinetics of C─C coupling often result low yield and poor selectivity for C Herein, performance Cu catalysts varying sizes is investigated, prepared via a cryo‐mediated liquid phase exfoliation technique, electrochemical to . The activity gradually increase as size decreases tens nanometers few nanometers. Impressively, 5 nm quantum dots (Cu‐5) achieve maximum Faradaic efficiency (FE) 81.5% half‐cell cathodic energy (CEE) 42.2% with large partial current density 1.1 A cm −2 at −0.93 V versus reversible hydrogen electrode. Structural characterization situ spectroscopic analysis reveal that Cu‐5 dots, dominated by (100) facet, provide an abundance active sites enhance adsorption activation, promoting formation *CO intermediates. accumulation intermediates on facilitates CO‐CHO reaction, thus enhancing production rate.

Language: Английский

Citations

15
Improved performances toward electrochemical carbon dioxide and oxygen reductions by iron-doped stannum nanoparticles DOI

Jiangtao Zhu,

Quan Zhang, Caiyun Wang

et al.

Nanoscale, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 1, 2025

We have designed a catalyst that can efficiently convert CO 2 into through Zn–CO batteries and the electrochemical RR, addressing both energy conversion environmental concerns simultaneously.

Language: Английский

Citations

2
Nitrogen-Rich Carbon Nanomaterials Embedded with Ni Nanoparticles for Electrochemical Carbon Dioxide Reduction DOI
Shengshen Gu,

Jiacheng Lu,

Xiuxiu Ren

et al.

ACS Applied Nano Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 21, 2025

Language: Английский

Citations

2
Toward Complete CO2 Electroconversion: Status, Challenges, and Perspectives DOI Creative Commons
Changfan Xu,

Ping Hong,

Yulian Dong

et al.

Advanced Energy Materials, Journal Year: 2025, Volume and Issue: unknown

Published: March 12, 2025

Abstract Electrocatalytic conversion of carbon dioxide (CO 2 ) into valuable carbon‐based fuels and chemicals represents a promising approach to closing the cycle setting circular economy. Nevertheless, for current electrocatalytic CO reduction reaction (ECO RR) systems, realizing 100% with simultaneously high overall rate (i.e., single‐pass conversion) Faradaic efficiency (FE) remains significant challenge. Enhancing often results in decrease FE, conversely, improving FE may limit rate. Metal–CO (M–CO batteries functions face similar challenges, particularly reversible M–CO batteries, which do not accomplish net because nearly all RR products are reoxidized during subsequent charging process. Such system neutrality poses substantial challenges. This perspective provides an in‐depth analysis state‐of‐the‐art ECO systems alongside main strategies employed address their respective The critical importance achieving both is underscored practical applications effectively close cycle. Furthermore, strategic roadmap that outlines future research directions presented, thereby facilitating advancement comprehensive electroconversion technologies.

Language: Английский

Citations

2
Catalyzed carbon-based materials for CO2-battery utilization DOI Open Access

Yulian Dong,

Changfan Xu, Yonghuan Fu

et al.

Energy Materials, Journal Year: 2025, Volume and Issue: 5(4)

Published: Jan. 23, 2025

Increasing atmospheric CO2 levels and global carbon neutrality goals have driven interest in technologies that both mitigate emissions provide sustainable energy storage solutions. Metal-carbon dioxide (M-CO2) batteries offer significant promise due to their high density potential utilize CO2. A key challenge advancing M-CO2 lies optimizing CO2-breathing cathodes, which are essential for adsorption, diffusion, conversion. Carbon-based cathodes play a critical role facilitating redox batteries, owing cost-effectiveness, conductivity, tunable microstructure, porosity. However, there is lack of current systematic understanding the relationship between structure, composition, catalytic properties carbon-based as well impact on overall efficiency, stability, durability batteries. In this review, we will give an insightful review analysis recent advances various materials, including commercial carbons, single-atom catalysts, transition metal/carbon composites, metal-organic frameworks, etc. , focusing structure-function-property relationships. comprehensive pivotal played by materials optimization strategies be provided. Moreover, future perspectives research suggestions presented advance development innovation

Language: Английский

Citations

1
Modulating Electronic Density of Single‐Atom Ni Center by Heteroatoms for Efficient CO2 Electroreduction DOI Open Access
Yang Chen, Xiaoli Pan, Lin Li

et al.

Small, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 24, 2025

Abstract Single‐atom catalysts (SACs) with unique geometric and electronic configurations have triggered great interest in many important reactions. However, controllably modulating the structure of metal centers to enhance catalytic performance remains a challenge. Here, Ni over 1 ‐NC SACs by introducing electron‐rich phosphorus or electron‐deficient boron for electrochemical CO 2 reduction (CO RR) is systematically tailored. It found that ‐PNC ‐N 3 P site exhibits superior current density 14.6 mA cm −2 Faradaic efficiency 90.6% at −0.8 V versus RHE production, far exceeding ‐BNC SACs. Detailed characterizations theoretical calculations reveal linear relationship between valence state species RR performance. The incorporation facilitates localization around center, significantly promoting adsorption formation key *COOH intermediate RR. This work provides feasible approach quantitatively manipulate single‐atom sites rationally design highly efficient boosted

Language: Английский

Citations

1
Enhanced pH-universal industrial-level CO2 reduction in N-doped carbon with nickel particles active sites via accelerated proton transport kinetics DOI

Haiqiang Mu,

Pengyue Shan, Ting Zhang

et al.

Carbon, Journal Year: 2025, Volume and Issue: unknown, P. 120096 - 120096

Published: Feb. 1, 2025

Language: Английский

Citations

1
Biological Neural Network‐Inspired Micro/Nano‐Fibrous Carbon Aerogel for Coupling Fe Atomic Clusters With Fe‐N4 Single Atoms to Enhance Oxygen Reduction Reaction DOI Open Access
Jiaojiao Sun, Mengxia Shen,

A. Jun Chang

et al.

Small, Journal Year: 2025, Volume and Issue: unknown

Published: March 5, 2025

Nitrogen-coordinated metal single atoms catalysts, especially with M-N4 configuration confined within the carbon matrix, emerge as a frontier of electrocatalytic research for enhancing sluggish kinetics oxygen reduction reaction (ORR). Nevertheless, due to highly planar D4h symmetry in M-N4, their adsorption behavior toward intermediates is limited, undesirably elevating energy barriers associated ORR. Moreover, structural engineering substrate also poses significant challenges. Herein, inspired by biological neural network (BNN), reticular nervous system high-speed signal processing and transmitting, comprehensive biomimetic strategy proposed tailoring Fe-N4 (Fe SAs) coupled Fe atomic clusters ACs) active sites, which are anchored onto chitosan microfibers/nanofibers-based aerogel (CMNCA-FeSA+AC) continuous conductive channels an oriented porous architecture. Theoretical analysis reveals synergistic effect SAs ACs optimizing electronic structures expediting The ingenious will shed light on topology optimization efficient electrocatalysts advanced electrochemical conversion devices.

Language: Английский

Citations

1
Concerted catalysis of single atom and nanocluster enhances bio-ethanol activation and dehydrogenation DOI Creative Commons
Zhao Sun,

Weizhi Shi,

Louise R. Smith

et al.

Nature Communications, Journal Year: 2025, Volume and Issue: 16(1)

Published: April 26, 2025

Language: Английский

Citations

1