Overcoming Electrostatic Interaction via Pulsed Electroreduction for Boosting the Electrocatalytic Urea Synthesis DOI
Weibin Qiu,

Shimei Qin,

Yibao Li

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(24)

Published: April 10, 2024

Abstract Electrocatalytic urea synthesis under ambient conditions offers a promising alternative strategy to the traditional energy‐intensive industry protocol. Limited by electrostatic interaction, reduction reaction of anions at cathode in electrocatalytic system is not easily achievable. Here, we propose novel overcome interaction via pulsed electroreduction. We found that reconstruction‐resistant CuSiO x nanotube, with abundant atomic Cu−O−Si interfacial sites, exhibits ultrastability electrosynthesis from nitrate and CO 2 . Under potential approach optimal operating conditions, interfaces achieve superior production rate (1606.1 μg h −1 mg cat. ) high selectivity (79.01 %) stability (the Faradaic efficiency retained 80 % even after testing), outperforming most reported catalysts. believe our will incite further investigation into electroreduction increasing substrate transport, which may guide design other energy conversion systems.

Language: Английский

Atomically dispersed materials: Ideal catalysts in atomic era DOI
Tao Gan, Dingsheng Wang

Nano Research, Journal Year: 2023, Volume and Issue: 17(1), P. 18 - 38

Published: May 25, 2023

Language: Английский

Citations

213
Synergistic Fe−Se Atom Pairs as Bifunctional Oxygen Electrocatalysts Boost Low‐Temperature Rechargeable Zn‐Air Battery DOI
Yao Wang, Jiao Wu, Shuaihao Tang

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(15)

Published: Feb. 18, 2023

Herein, we successfully construct bifunctional electrocatalysts by synthesizing atomically dispersed Fe-Se atom pairs supported on N-doped carbon (Fe-Se/NC). The obtained Fe-Se/NC shows a noteworthy oxygen catalytic performance with low potential difference of 0.698 V, far superior to that reported Fe-based single-atom catalysts. theoretical calculations reveal p-d orbital hybridization around the leads remarkably asymmetrical polarized charge distributions. based solid-state rechargeable Zn-air batteries (ZABs-Fe-Se/NC) present stable charge/discharge 200 h (1090 cycles) at 20 mA cm-2 25 °C, which is 6.9 times ZABs-Pt/C+Ir/C. At extremely temperature -40 ZABs-Fe-Se/NC displays an ultra-robust cycling 741 (4041 1 , about 11.7 More importantly, could be operated for 133 (725 even 5 °C.

Language: Английский

Citations

201
Dual‐Atom Support Boosts Nickel‐Catalyzed Urea Electrooxidation DOI
Xiaobo Zheng, Jiarui Yang, Peng Li

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(22)

Published: March 24, 2023

Nickel-based catalysts have been regarded as one of the most promising electrocatalysts for urea oxidation reaction (UOR), however, their activity is largely limited by inevitable self-oxidation Ni species (NSOR) during UOR. Here, we proposed an interface chemistry modulation strategy to trigger occurrence UOR before NSOR via constructing a 2D/2D heterostructure that consists ultrathin NiO anchored Ru-Co dual-atom support (Ru-Co DAS/NiO). Operando spectroscopic characterizations confirm this unique triggering mechanism on surface DAS/NiO. Consequently, fabricated catalyst exhibits outstanding with low potential 1.288 V at 10 mA cm-2 and remarkable long-term durability more than 330 h operation. DFT calculations demonstrate favorable electronic structure induced heterointerface endows energetically NSOR.

Language: Английский

Citations

197
Microenvironment Engineering of Single/Dual‐Atom Catalysts for Electrocatalytic Application DOI Open Access
Yun Gao, Baozhong Liu, Dingsheng Wang

et al.

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(31)

Published: Feb. 23, 2023

Single/dual-metal atoms supported on carbon matrix can be modulated by coordination structure and neighboring active sites. Precisely designing the geometric electronic uncovering structure-property relationships of single/dual-metal confront with grand challenges. Herein, this review summarizes latest progress in microenvironment engineering single/dual-atom sites via a comprehensive comparison single-atom catalyst (SACs) dual-atom catalysts (DACs) term design principles, modulation strategy, theoretical understanding structure-performance correlations. Subsequently, recent advances several typical electrocatalysis process are discussed to get general reaction mechanisms finely-tuned SACs DACs. Finally, full-scaled summaries challenges prospects given for This will provide new inspiration development atomically dispersed electrocatalytic application.

Language: Английский

Citations

181
The reformation of catalyst: From a trial-and-error synthesis to rational design DOI
Ligang Wang, Jiabin Wu,

Shunwu Wang

et al.

Nano Research, Journal Year: 2023, Volume and Issue: 17(4), P. 3261 - 3301

Published: Sept. 27, 2023

Language: Английский

Citations

181
Electrocatalytic water splitting: Mechanism and electrocatalyst design DOI
Han Wu,

Qiaoxian Huang,

Yuanyuan Shi

et al.

Nano Research, Journal Year: 2023, Volume and Issue: 16(7), P. 9142 - 9157

Published: April 2, 2023

Language: Английский

Citations

175
Liquid Fluxional Ga Single Atom Catalysts for Efficient Electrochemical CO2Reduction DOI
Zedong Zhang, Jiexin Zhu, Shenghua Chen

et al.

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 62(3)

Published: Nov. 18, 2022

Precise design and tuning of the micro-atomic structure single atom catalysts (SACs) can help efficiently adapt complex catalytic systems. Herein, we inventively found that when active center main group element gallium (Ga) is downsized to atomic level, whose characteristic has significant differences from conventional bulk rigid Ga catalysts. The SACs with a P, S coordination environment display specific flow properties, showing CO products FE ≈92 % at -0.3 V vs. RHE in electrochemical CO2 reduction (CO2 RR). Theoretical simulations demonstrate adaptive dynamic transition optimizes adsorption energy *COOH intermediate renews sites time, leading excellent RR selectivity stability. This liquid system interfaces lays foundation for future exploration synthesis catalysis.

Language: Английский

Citations

162
Continuous Modulation of Electrocatalytic Oxygen Reduction Activities of Single‐Atom Catalysts throughp‐nJunction Rectification DOI
Zechao Zhuang, Lixue Xia,

Jiazhao Huang

et al.

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 62(5)

Published: Nov. 16, 2022

Fine-tuning single-atom catalysts (SACs) to surpass their activity limit remains challenging at atomic scale. Herein, we exploit p-type semiconducting character of SACs having a metal center coordinated nitrogen donors (MeNx ) and rectify local charge density by an n-type semiconductor support. With iron phthalocyanine (FePc) as model SAC, introducing gallium monosulfide that features low work function generates space-charged region across the junction interface, causes distortion FeN4 moiety spin-state transition in FeII center. This catalyst shows over two-fold higher specific oxygen-reduction than pristine FePc. We further employ three other chalcogenides varying supports, discover linear correlation between activities supported rectification degrees, which clearly indicates can be continuously tuned this strategy.

Language: Английский

Citations

158
Construction of Co4 Atomic Clusters to Enable Fe−N4 Motifs with Highly Active and Durable Oxygen Reduction Performance DOI
Ali Han, Wenming Sun, Xin Wan

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(30)

Published: May 24, 2023

Abstract Fe−N−C catalysts with single‐atom Fe−N 4 configurations are highly needed owing to the high activity for oxygen reduction reaction (ORR). However, limited intrinsic and dissatisfactory durability have significantly restrained practical application of proton‐exchange membrane fuel cells (PEMFCs). Here, we demonstrate that constructing adjacent metal atomic clusters (ACs) is effective in boosting ORR performance stability catalysts. The integration uniform Co ACs on N‐doped carbon substrate (Co @/Fe 1 @NC) realized through a “pre‐constrained” strategy using molecular Fe(acac) 3 implanted precursors. as‐developed @NC catalyst exhibits excellent half‐wave potential ( E 1/2 ) 0.835 V vs. RHE acidic media peak power density 840 mW cm −2 H 2 −O cell test. First‐principles calculations further clarify catalytic mechanism identified modified ACs. This work provides viable precisely establishing atomically dispersed polymetallic centers efficient energy‐related catalysis.

Language: Английский

Citations

149
Tuning Mass Transport in Electrocatalysis Down to Sub‐5 nm through Nanoscale Grade Separation DOI
Zhenhui Liu, Yue Du, Ruohan Yu

et al.

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 62(3)

Published: Nov. 18, 2022

Nano and single-atom catalysis open new possibilities of producing green hydrogen (H2 ) by water electrolysis. However, for the evolution reaction (HER) which occurs at a characteristic rate proportional to potential, fast generation H2 nanobubbles atomic-scale interfaces often leads blockage active sites. Herein, nanoscale grade-separation strategy is proposed tackle mass-transport problem utilizing ordered three-dimensional (3d) interconnected sub-5 nm pores. The results reveal that 3d criss-crossing mesopores with grade separation allow efficient diffusion bubbles along channels. After support ultrafine ruthenium (Ru), are on superior level two-dimensional system maximizing catalyst performance obtained Ru outperforms most other HER catalysts. This work provides potential route fine-tuning few-nanometer mass transport during

Language: Английский

Citations

137