A General Strategy Based on Hetero‐Charge Coupling Effect for Constructing Single‐Atom Sites DOI
Cheng Peng, Mingyue Wang, Sha Li

et al.

Angewandte Chemie, Journal Year: 2024, Volume and Issue: 136(36)

Published: June 17, 2024

Abstract Single‐atom catalysts have emerged as cutting‐edge hotspots in the field of material science owing to their excellent catalytic performance brought about by well‐defined metal single‐atom sites (M SASs). However, huge challenges still lie achieving rational design and precise synthesis M SASs. Herein, we report a novel strategy based on hetero‐charge coupling effect (HCCE) prepare SASs loaded N S co‐doped porous carbon 1 /NSC). The proposed was widely applied 17 types /NSC composed single or multi‐metal with integrated regulation coordination environment electronic structure, exhibiting good universality flexible adjustability. Furthermore, this provided low‐cost method efficiently synthesizing high yields, that can produce more than 50 g catalyst at one time, which is key large‐scale production. Among various as‐prepared unary be Fe, Co, Ni, V, Cr, Mn, Mo, Pd, W, Re, Ir, Pt, Bi) catalysts, Fe delivered for electrocatalytic nitrate reduction NH 3 Faradaic efficiency 86.6 % yield rate 1.50 mg h −1 cat. −0.6 V vs. RHE. Even using cathode Zn‐nitrate battery, it exhibited open circuit voltage 1.756 energy density 4.42 mW cm −2 cycling stability.

Language: Английский

Revealing the Active Sites in Atomically Dispersed Multi‐Metal–Nitrogen–Carbon Catalysts DOI

Buwei Sun,

Shiyu Zhang, Haozhou Yang

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(29)

Published: Jan. 30, 2024

Abstract Atomically dispersed metal‐nitrogen‐carbon catalysts have been extensively explored for various sustainable energy‐related reactions. From a material perspective, these are likely to consist of combination single‐atom, dual‐atom and possibly even multi‐atom sites. However, pinpointing their true active sites has remained challenging task. In this study, model catalyst is introduced, Co/CoMn‐NC, featuring both Co single‐atom CoMn on nitrogen‐doped carbon substrate. By employing X‐ray adsorption spectroscopy density functional theory calculations, the atomic configuration Co/CoMn‐NC determined. Density calculations also used unequivocally identify Co‐atom within motif as predominate site toward oxygen reduction reaction (ORR), which further confirmed by in situ Raman spectroscopy. The cooperative interactions between can finely tune d‐band center ameliorate desorption behaviors intermediates, thereby facilitating ORR kinetic. Overall, study introduces systematic strategy elucidate structure superiority system provides new insights into atomically multi‐metal sites, showcasing that enhanced catalytic performance extends beyond unified diatomic or monatomic

Language: Английский

Citations

25
Oxygen-bridging Fe, Co dual-metal dimers boost reversible oxygen electrocatalysis for rechargeable Zn–air batteries DOI Creative Commons
Qixing Zhou, Wendan Xue, Xun Cui

et al.

Proceedings of the National Academy of Sciences, Journal Year: 2024, Volume and Issue: 121(30)

Published: July 18, 2024

Rechargeable zinc–air batteries (ZABs) are regarded as a remarkably promising alternative to current lithium-ion batteries, addressing the requirements for large-scale high-energy storage. Nevertheless, sluggish kinetics involving oxygen reduction reaction (ORR) and evolution (OER) hamper widespread application of ZABs, necessitating development high-efficiency durable bifunctional electrocatalysts. Here, we report atom–bridged Fe, Co dual-metal dimers (FeOCo-SAD), in which active site Fe–O–Co–N 6 moiety boosts exceptional reversible activity toward ORR OER alkaline electrolytes. Specifically, FeOCo-SAD achieves half-wave potential ( E 1/2 ) 0.87 V an overpotential 310 mV at density 10 mA cm –2 OER, with gap (Δ only 0.67 V. Meanwhile, manifests high performance peak power 241.24 mW −2 realistic rechargeable ZABs. Theoretical calculations demonstrate that introduction bridge dimer induced charge spatial redistribution around Fe atoms. This enhances activation optimizes adsorption/desorption dynamics intermediates. Consequently, energy barriers effectively reduced, leading strong promotion intrinsic OER. work suggests oxygen-bridging offer prospects significantly enhancing electrocatalysis creating innovative catalysts exhibit synergistic effects electronic states.

Language: Английский

Citations

19
Recent progress in the synthesis of N-substituted arylamines by reductive cross-coupling of nitroarenes DOI

Jing‐Hao Qin,

Wang Yao,

Jun-Yao Ouyang

et al.

Organic Chemistry Frontiers, Journal Year: 2024, Volume and Issue: 11(9), P. 2638 - 2664

Published: Jan. 1, 2024

This review describes the recent advances in different reaction types and catalytic systems for construction of C–NAr S–NAr bonds by nitroaromatic reductive cross-coupling.

Language: Английский

Citations

11
Multicomponent Reductive Coupling for Selective Access to Functional γ-Lactams by a Single-Atom Cobalt Catalyst DOI
Jialu Sun, Huanfeng Jiang, Pierre H. Dixneuf

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: unknown

Published: March 21, 2024

Despite their significant importance to numerous fields, the difficulties in direct and diverse synthesis of α-hydroxy-γ-lactams pose substantial obstacles practical applications. Here, we designed a nitrogen TiO2 co-doped graphitic carbon-supported material with atomically dispersed cobalt sites (CoSA-N/NC-TiO2), which was successfully applied as multifunctional catalyst establish general method for construction from cheap abundant nitro(hetero)arenes, aldehydes, H2O alkynoates. The striking features operational simplicity, broad substrate functionality compatibility (>100 examples), high step atom efficiency, good selectivity, exceptional reusability highlight practicality this new catalytic transformation. Mechanistic studies reveal that active CoN4 species dopants exhibit synergistic effect on formation key acid-masked nitrones; subsequent nucleophilic addition alkynoates followed by successive reduction, alkenyl hydration, intramolecular ester ammonolysis delivers desired products. In work, concept reduction interruption leading reaction route will open door further develop useful transformations rational design.

Language: Английский

Citations

9
Harnessing Atomically Dispersed Cobalt for the Reductive Catalytic Fractionation of Lignocellulose DOI Creative Commons
Xiancheng Li,

Rumin Ma,

Xueying Gao

et al.

Advanced Science, Journal Year: 2024, Volume and Issue: 11(22)

Published: March 17, 2024

Abstract The reductive catalytic fractionation (RCF) of lignocellulose, considering lignin valorization at design time, has demonstrated the entire utilization all lignocellulose components; however, such processes always require catalysts based on precious metals or high‐loaded nonprecious metals. Herein, study develops an ultra‐low loaded, atomically dispersed cobalt catalyst, which displays exceptional performance in RCF lignocellulose. An approximately theoretical maximum yield phenolic monomers (48.3 wt.%) from is realized, rivaling metal catalysts. High selectivity toward 4‐propyl‐substituted guaiacol/syringol facilitates their purification and follows syntheses highly adhesive polyesters. Lignin nanoparticles (LNPs) are generated by simple treatment obtained dimers oligomers. RCF‐resulted carbohydrate pulp more obedient to enzymatic hydrolysis. Experimental studies model compounds reveal concerted cleavage C α –O β pathway for rupture β‐O‐4 structure. Overall, approach involves valorizing products derived biopolymer, providing opportunity comprehensive components within

Language: Английский

Citations

8
Direct C−C Double Bond Cleavage of Alkenes Enabled by Highly Dispersed Cobalt Catalyst and Hydroxylamine DOI
Wenxuan Xue, Yijie Jiang, Hongcheng Lu

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(52)

Published: Nov. 15, 2023

The utilization of a single-atom catalyst to break C-C bonds merges the merits homogeneous and heterogeneous catalysis presents an intriguing pathway for obtaining high-value-added products. Herein, mild, selective, sustainable oxidative cleavage alkene form oxime ether or nitrile was achieved by using atomically dispersed cobalt hydroxylamine. Diversified substrate patterns, including symmetrical unsymmetrical alkenes, di- tri-substituted late-stage functionalization complex alkenes were demonstrated. reaction successfully scaled up demonstrated good performance in recycling experiments. hot filtration test, poisoning radical scavenger experiment, time kinetics, studies on intermediate collectively pointed mechanism with cobalt/acid/O2 promoted bond as key step.

Language: Английский

Citations

17
Synergistic Pore Structure and Active Site Modulation in Co–N–C Catalysts Enabling Stable Zinc–Air Batteries DOI

Xushan Li,

Xiaowei Lv,

Panpan Sun

et al.

ACS Applied Materials & Interfaces, Journal Year: 2024, Volume and Issue: 16(23), P. 29979 - 29990

Published: May 30, 2024

Development of cheap, highly active, and durable nonprecious metal-based oxygen electrocatalysts is essential for metal–air battery technology, but achieving the balance evolution reaction (OER)/oxygen reduction (ORR) bifunctional performance long-term durability still a great challenge. Using typical Co–N–C catalyst as model, herein, we introduced ammonium chloride into nitrogen-doped carbon materials containing metal elements during pyrolysis process (Co–N–C/AC), which not only increases active area also realizes accurate customization site (pyridine nitrogen cobalt oxide species) so to achieve OER/ORR sites. The synthesized Co–N–C/AC with three-dimensional porous structure exhibits smaller potential gap 0.72 V. peak power density aqueous cell at current 308 mA cm–2 203 mW cm–2. cycle life (≈3900 h) longer than those other recently reported Zn–air batteries (ZABs). Co–N–C/AC-based quasi-solid-state ZAB reaches 550 ∼72 h. This work shows feasible path practical application ZABs by balancing tailoring reasonably.

Language: Английский

Citations

7
Advancing Heterogeneous Organic Synthesis With Coordination Chemistry‐Empowered Single‐Atom Catalysts DOI

Bo‐Chao Ye,

Wenhao Li, Xia Zhang

et al.

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

Published: Sept. 18, 2024

Abstract For traditional metal complexes, intricate chemistry is required to acquire appropriate ligands for controlling the electron and steric hindrance of active centers. Comparatively, preparation single‐atom catalysts much easier with more straightforward effective accesses arrangement control The presence coordination atoms or neighboring functional on supports' surface ensures stability single‐atoms their interactions individual substantially regulate performance Therefore, collaborative interaction between surrounding environment enhances initiation reaction substrates formation transformation crucial intermediate compounds, which imparts significant catalytic efficacy, rendering them a valuable framework investigating correlation structure activity, as well mechanism in organic reactions. Herein, comprehensive overviews both homogeneous complexes reactions are provided. Additionally, reflective conjectures about advancement synthesis also proposed present reference later development.

Language: Английский

Citations

6
Multi-hydroxyl POSS supported iridium complexes as a recyclable catalyst for selective synthesis of N-/C-substituted indoles and the total synthesis of HIV-1 fusion inhibitor DOI
Jiahao Li, Li Chen, Likui Wang

et al.

Journal of Catalysis, Journal Year: 2023, Volume and Issue: 429, P. 115205 - 115205

Published: Nov. 24, 2023

Language: Английский

Citations

12
Preparation of reusable copper-based biomass-carbon aerogel catalysts and their application in highly selective reduction of maleimides to succinimides with hydrosilane as a hydrogen source DOI

Shaohuan Lv,

Zhanhong Yuan,

Juanjuan Zheng

et al.

Green Chemistry, Journal Year: 2024, Volume and Issue: 26(5), P. 2592 - 2598

Published: Jan. 1, 2024

A novel copper-based biomass-carbon aerogel catalyst was prepared as a highly efficient and selective for maleimides reduction the first time with excellent catalytic activity, chemo-selectivity, recyclability.

Language: Английский

Citations

4