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

Bo‐Chao Ye,

Wenhao Li, Xia Zhang

и другие.

Advanced Materials, Год журнала: 2024, Номер unknown

Опубликована: Сен. 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.

Язык: Английский

Designing 3d Transition Metal Cation-Doped MRuOx As Durable Acidic Oxygen Evolution Electrocatalysts for PEM Water Electrolyzers DOI
Panpan Sun, Zelong Qiao,

Xiaobin Dong

и другие.

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(22), С. 15515 - 15524

Опубликована: Май 24, 2024

The continuous dissolution and oxidation of active sites in Ru-based electrocatalysts have greatly hindered their practical application proton exchange membrane water electrolyzers (PEMWE). In this work, we first used density functional theory (DFT) to calculate the energy Ru 3d transition metal-doped MRuOx (M = Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn) evaluate stability for acidic oxygen evolution reaction (OER) screen out ZnRuOx as best candidate. To confirm theoretical predictions, experimentally synthesized these materials found that indeed displays robust OER with a negligible decay η10 after 15 000 CV cycles. Of importance, using anode, PEMWE can run stably 120 h at 200 mA cm–2. We also further uncover mechanism ZnRuOx, i.e., Zn atoms doped outside nanocrystal would form "Zn-rich" shell, which effectively shortened average Ru–O bond lengths strengthen interaction therefore boosted intrinsic OER. short, work not only provides new study paradigm DFT calculations guide experimental synthesis but offers proof-of-concept metal dopants RuO2 stabilizer universal principle develop high-durability catalysts PEMWE.

Язык: Английский

Процитировано

60
General Design Concept of High‐Performance Single‐Atom‐Site Catalysts for H2O2 Electrosynthesis DOI

Mingyang Deng,

Dingsheng Wang, Yadong Li

и другие.

Advanced Materials, Год журнала: 2024, Номер 36(24)

Опубликована: Март 5, 2024

Hydrogen peroxide (H

Язык: Английский

Процитировано

27
Challenges and Opportunities for Single‐Atom Electrocatalysts: From Lab‐Scale Research to Potential Industry‐Level Applications DOI Creative Commons
Chen Jia, Qian Sun, Ruirui Liu

и другие.

Advanced Materials, Год журнала: 2024, Номер unknown

Опубликована: Июнь 13, 2024

Single-atom electrocatalysts (SACs) are a class of promising materials for driving electrochemical energy conversion reactions due to their intrinsic advantages, including maximum metal utilization, well-defined active structures, and strong interface effects. However, SACs have not reached full commercialization broad industrial applications. This review summarizes recent research achievements in the design crucial electrocatalytic on sites, coordination, substrates, as well synthesis methods. The key challenges facing activity, selectivity, stability, scalability, highlighted. Furthermore, it is pointed out new strategies address these increasing activity enhancing utilization improving optimizing local environment, developing fabrication techniques, leveraging insights from theoretical studies, expanding potential Finally, views offered future direction single-atom electrocatalysis toward commercialization.

Язык: Английский

Процитировано

26
Atomically dispersed multi-site catalysts: bifunctional oxygen electrocatalysts boost flexible zinc–air battery performance DOI
Shengchen Wang, Mengyang Zhang,

Xueqin Mu

и другие.

Energy & Environmental Science, Год журнала: 2024, Номер 17(14), С. 4847 - 4870

Опубликована: Янв. 1, 2024

Based on the advancements in atomically dispersed multi-site catalysts for FZABs, this review discusses design methodologies to regulate performance of bifunctional oxygen electrocatalysts from electronic and geometric structures.

Язык: Английский

Процитировано

21
Lignin-based support for metal catalysts: Synthetic strategies, performance boost, and application advances DOI

Tairan Pang,

Guanhua Wang,

Wenjie Sui

и другие.

Coordination Chemistry Reviews, Год журнала: 2025, Номер 528, С. 216426 - 216426

Опубликована: Янв. 10, 2025

Язык: Английский

Процитировано

6
Destabilization of Single‐Atom Catalysts: Characterization, Mechanisms, and Regeneration Strategies DOI Open Access

Zhiquan Lang,

Xixi Wang,

Sobia Jabeen

и другие.

Advanced Materials, Год журнала: 2025, Номер unknown

Опубликована: Янв. 19, 2025

Abstract Numerous in situ characterization studies have focused on revealing the catalytic mechanisms of single‐atom catalysts (SACs), providing a theoretical basis for their rational design. Although research is relatively limited, stability SACs under long‐term operating conditions equally important and prerequisite real‐world energy applications, such as fuel cells water electrolyzers. Recently, there has been rise destabilization regeneration SACs; however, timely comprehensive summaries that provide catalysis community with valuable insights directions are still lacking. This review summarizes recent advances strategies SACs, specifically highlighting various state‐of‐the‐art techniques employed studies. The factors induce identified by discussing failure active sites, coordination environments, supports, reaction scenarios. Next, primary introduced, including redispersion, surface poison desorption, exposure subsurface sites. Additionally, advantages limitations both ex discussed. Finally, future proposed, aimed at constructing structure–stability relationships guiding design more stable SACs.

Язык: Английский

Процитировано

4
Highly Selective Electrochemical Baeyer–Villiger Oxidation through Oxygen Atom Transfer from Water DOI
Yu Mu, Boqiang Chen, Hongna Zhang

и другие.

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(19), С. 13438 - 13444

Опубликована: Апрель 30, 2024

The Baeyer–Villiger oxidation of ketones is a crucial oxygen atom transfer (OAT) process used for ester production. Traditionally, accomplished by thermally oxidizing the OAT from stoichiometric peroxides, which are often difficult to handle. Electrochemical methods hold promise breaking limitation using water as source. Nevertheless, existing demonstrations electrochemical face challenges low selectivity. We report in this study strategy overcome challenge. By employing well-known catalyst, Fe2O3, we achieved nearly perfect selectivity cyclohexanone. Mechanistic studies suggest that it essential produce surface hydroperoxo intermediates (M-OOH, where M represents metal center) promote nucleophilic attack on ketone substrates. confining reactions catalyst surfaces, competing (e.g., dehydrogenation, carboxylic acid cation rearrangements, and hydroxylation) greatly limited, thereby offering high surface-initiated nature reaction confirmed kinetic spectroelectrochemical characterizations. This discovery adds toolbox organic synthesis.

Язык: Английский

Процитировано

15
Deciphering Cationic and Anionic Overoxidation: Key Insights into the Intrinsic Structural Degradation of Catalysts DOI
Xiaobo Zheng, Jiarui Yang, Xun Xu

и другие.

Advanced Energy Materials, Год журнала: 2024, Номер 14(30)

Опубликована: Май 14, 2024

Abstract Proton exchange membrane water electrolyzer (PEMWE) technology holds tremendous promise for large‐scale green hydrogen production. However, its widespread application faces significant constraints due to the limited lifespan of oxygen evolution reaction (OER) catalyst in highly acidic and oxidative operating environments. Therefore, a comprehensive understanding catalyst's structural degradation mechanism is imperative rational design high‐performance catalysts. In this review, essence catalysts: irreversible cationic anionic overoxidation initially unveiled. This followed by an in‐depth exploration their intricate relationship with adsorbate (AEM) lattice oxidation (LOM). Then, state‐of‐the‐art characterization techniques analysis are introduced. Subsequently, 4 cutting‐edge antioxidation strategies, including heterostructure engineering, doping strategy, nanostructuring, phase engineering systematically discussed, aiming reveal intrinsic factors effectively inhibiting overoxidation. Finally, remaining challenges prospective insights into catalysts PEMWE delineated. The overarching goal review facilitate fundamental mechanisms provide principal guidelines robust OER

Язык: Английский

Процитировано

14
Precise synthesis of dual atom sites for electrocatalysis DOI
Yao Wang,

Fengya Ma,

Guoqing Zhang

и другие.

Nano Research, Год журнала: 2024, Номер unknown

Опубликована: Сен. 17, 2024

Язык: Английский

Процитировано

13
Multicomponent Reductive Coupling for Selective Access to Functional γ-Lactams by a Single-Atom Cobalt Catalyst DOI
Jialu Sun, Huanfeng Jiang, Pierre H. Dixneuf

и другие.

Journal of the American Chemical Society, Год журнала: 2024, Номер unknown

Опубликована: Март 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.

Язык: Английский

Процитировано

9