Single-atom catalysts: promotors of highly sensitive and selective sensors DOI
Zehui Li, Enze Tian, Shunli Wang

et al.

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(15), P. 5088 - 5134

Published: Jan. 1, 2023

Sensors, the underlying technology that supports Internet of Things, are undergoing multi-disciplinary integration development to constantly improve efficiency human production and life. Simultaneously, application scenarios in emerging fields such as medical diagnosis, environmental monitoring industrial safety put forward higher requirements for sensing capabilities. Over last decade, single-atom catalysts (SACs) have attracted tremendous attention environment energy due their high atom utilization efficiencies, controllable active sites, tailorable coordination environments structural/chemical stability. These extraordinary characteristics extend sensitivity selectivity sensors beyond current limitations. Here, we start with working principles SAC-based sensors, summarize relationship between sensor performance intrinsic properties SACs, followed by an overview design strategy development. We then review recent advances different highlight future opportunities challenges exciting applications.

Language: Английский

Electrochemical Nitrate Reduction: Ammonia Synthesis and the Beyond DOI
Yuecheng Xiong, Yunhao Wang, Jingwen Zhou

et al.

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(17)

Published: June 9, 2023

Natural nitrogen cycle has been severely disrupted by anthropogenic activities. The overuse of N-containing fertilizers induces the increase nitrate level in surface and ground waters, substantial emission oxides causes heavy air pollution. Nitrogen gas, as main component air, used for mass ammonia production over a century, providing enough nutrition agriculture to support world population increase. In last decade, researchers have made great efforts develop processes under ambient conditions combat intensive energy consumption high carbon associated with Haber-Bosch process. Among different techniques, electrochemical reduction reaction (NO

Language: Английский

Citations

214
Single‐Atom Catalysis in Organic Synthesis DOI Creative Commons
Vitthal B. Saptal, Vincenzo Ruta, Mark A. Bajada

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(34)

Published: March 15, 2023

Single-atom catalysts hold the potential to significantly impact chemical sector, pushing boundaries of catalysis in new, uncharted directions. These materials, featuring isolated metal species ligated on solid supports, can exist many coordination environments, all which have shown important functions specific transformations. Their emergence has also provided exciting opportunities for mimicking metalloenzymes and bridging gap between homogeneous heterogeneous catalysis. This Review outlines impressive progress made recent years regarding use single-atom organic synthesis. We illustrate knowledge gaps search more sustainable, earth-abundant synthetic applications.

Language: Английский

Citations

111
Atomic coordination environment engineering of bimetallic alloy nanostructures for efficient ammonia electrosynthesis from nitrate DOI Creative Commons
Yunhao Wang, Mingzi Sun, Jingwen Zhou

et al.

Proceedings of the National Academy of Sciences, Journal Year: 2023, Volume and Issue: 120(32)

Published: July 31, 2023

Electrochemical nitrate reduction reaction (NO 3 RR) to ammonia has been regarded as a promising strategy balance the global nitrogen cycle. However, it still suffers from poor Faradaic efficiency (FE) and limited yield rate for production on heterogeneous electrocatalysts, especially in neutral solutions. Herein, we report one-pot synthesis of ultrathin nanosheet-assembled RuFe nanoflowers with low-coordinated Ru sites enhance NO RR performances electrolyte. Significantly, exhibit outstanding FE 92.9% 38.68 mg h −1 cat (64.47 ) at −0.30 −0.65 V (vs. reversible hydrogen electrode), respectively. Experimental studies theoretical calculations reveal that are highly electroactive an increased d-band center guarantee efficient electron transfer, leading low energy barriers reduction. The demonstration rechargeable zinc-nitrate batteries large-specific capacity using indicates their great potential next-generation electrochemical systems.

Language: Английский

Citations

104
Electrocatalytic Synthesis of Essential Amino Acids from Nitric Oxide Using Atomically Dispersed Fe on N‐doped Carbon DOI

Jiahui Xian,

Suisheng Li,

Hui Su

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(26)

Published: April 19, 2023

How to transfer industrial exhaust gases of nitrogen oxides into high-values product is significantly important and challenging. Herein, we demonstrate an innovative method for artificial synthesis essential α-amino acids from nitric oxide (NO) by reacting with α-keto through electrocatalytic process atomically dispersed Fe supported on N-doped carbon matrix (AD-Fe/NC) as the catalyst. A yield valine 32.1 μmol mgcat-1 delivered at -0.6 V vs. reversible hydrogen electrode, corresponding a selectivity 11.3 %. In situ X-ray absorption fine structure synchrotron radiation infrared spectroscopy analyses show that NO source converted hydroxylamine promptly nucleophilic attacked electrophilic center acid form oxime subsequent reductive hydrogenation occurred way amino acid. Over 6 kinds have been successfully synthesized gaseous can be also replaced liquid (NO3- ). Our findings not only provide creative converting high-valued products, which epoch-making significance towards acids, but benefit in deploying near-zero-emission technologies global environmental economic development.

Language: Английский

Citations

98
Interfacial engineering of transition metal dichalcogenide/carbon heterostructures for electrochemical energy applications DOI
Biao Chen, Simi Sui, Fang He

et al.

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(22), P. 7802 - 7847

Published: Jan. 1, 2023

This review provides a fundamental understanding of three types interfacial engineering in TMDC/C heterostructures and guidance for designing electrochemical energy applications.

Language: Английский

Citations

63
Phase Engineering of High‐Entropy Alloy for Enhanced Electrocatalytic Nitrate Reduction to Ammonia DOI
Rong Zhang, Yaqin Zhang, Bo Xiao

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(35)

Published: May 4, 2024

Abstract Directly electrochemical conversion of nitrate (NO 3 − ) is an efficient and environmentally friendly technology for ammonia (NH production but challenged by highly selective electrocatalysts. High‐entropy alloys (HEAs) with unique properties are attractive materials in catalysis, particularly multi‐step reactions. Herein, we first reported the application HEA (FeCoNiAlTi) electrocatalytic NO reduction to NH (NRA). The bulk active NRA limited unsatisfied yield 0.36 mg h −1 cm −2 Faradaic efficiency (FE) 82.66 %. Through effective phase engineering strategy, uniform intermetallic nanoparticles introduced on increase surface area charge transfer efficiency. resulting nanostructured (n‐HEA) delivers enhanced performance terms (0.52 FE (95.23 %). Further experimental theoretical investigations reveal that multi‐active sites (Fe, Co, Ni) dominated electrocatalysis over n‐HEA. Notably, typical Co exhibit lowest energy barrier *NH 2 as rate‐determining step.

Language: Английский

Citations

52
Photo-induced synthesis of heteronuclear dual-atom catalysts DOI
Qiuping Zhao, Wenxiong Shi, Jiangwei Zhang

et al.

Nature Synthesis, Journal Year: 2024, Volume and Issue: 3(4), P. 497 - 506

Published: Feb. 29, 2024

Language: Английский

Citations

50
Microwave‐Assisted Rapid Synthesis of MOF‐Based Single‐Atom Ni Catalyst for CO2 Electroreduction at Ampere‐Level Current DOI
Ming Wen, Nana Sun, Long Jiao

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(10)

Published: Jan. 17, 2024

Carbon-based single-atom catalysts (SACs) have attracted tremendous interest in heterogeneous catalysis. However, the common electric heating techniques to produce carbon-based SACs usually suffer from prolonged time and tedious operations. Herein, a general facile microwave-assisted rapid pyrolysis method is developed afford within 3 min without inert gas protection. The obtained present high porosity comparable carbonization degree those by techniques. Specifically, Ni implanted N-doped carbon (Ni

Language: Английский

Citations

48
Vanadium- and manganese-based metal-organic frameworks for potential environmental and catalysis applications DOI
Yangdan Pan,

Soheila Sanati,

Reza Abazari

et al.

Coordination Chemistry Reviews, Journal Year: 2024, Volume and Issue: 522, P. 216231 - 216231

Published: Sept. 25, 2024

Language: Английский

Citations

41
Single‐Atom Iron Catalyst as an Advanced Redox Mediator for Anodic Oxidation of Organic Electrosynthesis DOI

Xin‐Yu Wang,

Yong‐Zhou Pan,

Jiarui Yang

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(27)

Published: April 23, 2024

Homogeneous electrocatalysts can indirect oxidate the high overpotential substrates through single-electron transfer on electrode surface, enabling efficient operation of organic electrosynthesis catalytic cycles. However, problems this chemistry still exist such as dosage, difficult recovery, and low efficiency. Single-atom catalysts (SACs) exhibit atom utilization excellent activity, hold great promise in addressing limitations homogeneous catalysts. In view this, we have employed Fe-SA@NC an advanced redox mediator to try change situation. was synthesized using encapsulation-pyrolysis method, it demonstrated remarkable performance a range reported reactions, construction various C-C/C-X bonds. Moreover, potential exploring new synthetic method for electrosynthesis. We develop electro-oxidative ring-opening transformation cyclopropyl amides. reaction system, showed good tolerance drug molecules with complex structures, well flow electrochemical syntheses gram-scale transformations. This work highlights SACs electrosynthesis, thereby opening avenue chemistry.

Language: Английский

Citations

28