Nature Communications
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2024
·Vol. 15
·期 1
·1-12
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IF 14.7
Meng Yan,Liu Yu-Qin,Wang Chao,Si Yang,Wang Yun-Jie,Xia Wen-Qi,Liu Tian,Cao Xu,Guo Zhi-Yan,Chen Jie-Jie,Li Wen-Wei
The introduction of single-atom catalysts (SACs) into Fenton-like oxidation promises ultrafast water pollutant elimination, but the limited access to pollutants and oxidant by surface catalytic sites and the intensive oxidant consumption still severely restrict the decontamination performance. While nanoconfinement of SACs allows drastically enhanced decontamination reaction kinetics, the detailed regulatory mechanisms remain elusive. Here, we unveil that, apart from local enrichment of reactants, the catalytic pathway shift is also an important cause for the reactivity enhancement of nanoconfined SACs. The surface electronic structure of cobalt site is altered by confining it within the nanopores of mesostructured silica particles, which triggers a fundamental transition from singlet oxygen to electron transfer pathway for 4-chlorophenol oxidation. The changed pathway and accelerated interfacial mass transfer render the nanoconfined system up to 34.7-fold higher pollutant degradation rate and drastically raised peroxymonosulfate utilization efficiency (from 61.8% to 96.6%) relative to the unconfined control. It also demonstrates superior reactivity for the degradation of other electron-rich phenolic compounds, good environment robustness, and high stability for treating real lake water. Our findings deepen the knowledge of nanoconfined catalysis and may inspire innovations in low-carbon water purification technologies and other heterogeneous catalytic applications.
研究领域:
环境科学
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催化
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材料科学
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水处理
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DOI
PubMed
高影响因子
Carbon Energy
·
2022
·Vol. 5
·期 2
·e216
·
IF 21.556
Jiapeng Ji,Yunpeng Hou,Shiyu Zhou,Tong Qiu,Liang Zhang,Lu Ma,Chao Qian,Shaodong Zhou,Chengdu Liang,Min Ling
The oxygen evolution reaction (OER) activity of single-atom catalysts (SACs) is closely related to the coordination environment of the active site. Oxygen-coordinated atomic metal species bring about unique features beyond nitrogen-coordinated atomic metal species due to the fact that the M–O bond is weaker than the M–N bond. Herein, a series of metal–oxygen–carbon structured low-nucleus clusters (LNCs) are successfully anchored on the surface of multiwalled carbon nanotubes (M-MWCNTs, M = Ni, Co, or Fe) through a foolproof low-temperature gas transfer (300°C) method without any further treatment. The morphology and coordination configuration of the LNCs at the atomic level were confirmed by comprehensive characterizations. The synthetic Ni-MWCNTs electrocatalyst features excellent OER activity and stability under alkaline conditions, transcending the performances of Co-MWCNTs, Fe-MWCNTs and RuO 2 . Density functional theory calculations reveal that the moderate oxidation of low-nucleus Ni clusters changes the unoccupied orbital of Ni atoms, thereby lowering the energy barrier of the OER rate-limiting step and making the OER process more energy-efficient. This study demonstrates a novel versatile platform for large-scale manufacturing of oxygen-coordinated LNC catalysts.
研究领域:
催化
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电化学
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材料科学
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DOI
高影响因子
FOOD CHEMISTRY
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2025
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IF 9.8
Yanyan Cao,Meng Tao,Anan Xu,Zheng Tu,Shanshan Wang,Qinyan Yu,Sixu Li,Zhengquan Liu
Black tea contains sweet aroma compounds (SACs) with sweetening potential. However, a systematic understanding of their composition, enhancing effects, and underlying mechanisms is lacking. This study identified 14 key SACs in global sweet-aroma black teas using headspace solid-phase microextraction coupled with gas chromatography–mass spectrometry. Electronic tongue and sensory validation confirmed their sweetness-enhancing effects in a sugar-free black tea beverage and revealed their inherent taste properties (sweetness, astringency, pungency, and cooling). Molecular docking and dynamics simulation elucidated the stable bindings of T1R2/T1R3-benzeneacetaldehyde/ β -damascenone, α -amylase-benzeneacetaldehyde, TRPV1-geraniol, and TRPM8-methyl salicylate, mediated by hydrogen bonding and hydrophobic interactions. These protein-ligand complexes were proposed to modulate sweetness, sweet aftertaste, heat-evoked sweetness, and cooling-enhanced sweetness, respectively. Consequently, this study demonstrates that SACs enhance sweetness through cross-modal interactions and inherent taste properties, providing novel mechanistic insights and actionable strategies for flavor optimization in tea beverages and other food products.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Mengxia Shen,Qingqing Liu,Jiaojiao Sun,Chanjuan Liang,Chuanyin Xiong,Chen Hou,Jianfeng Huang,Liyun Cao,Yongqiang Feng,Zhen Shang
Single-atom catalysts (SACs), with precisely controlled metal atom distribution and adjustable coordination architecture, have gained intensive concerns as efficient oxygen reduction reaction (ORR) electrocatalysts in Zn-air batteries (ZAB). The attainment of a monodispersed state for metallic atoms anchored on the carbonaceous substrate remains the foremost research priority; however, the persistent challenges lie in the relatively weak metal-support interactions and the instability of captured single atom active sites. Furthermore, in order to achieve rapid transport of O 2 and other reactive substances within the carbon matrix, manufacturing SACs based on multi-stage porous carbon substrates is highly anticipated. Here, we propose a methodology for the fabrication of carbon aerogels (CA)-supported SACs utilizing papermaking nanofibers , which incorporates advanced strategies for N -atom self-doping, defect/vacancy introduction, and single-atom interface engineering. Specifically, taking advantages of using green and energy-efficient feedstocks, combining with a direct pore-forming template volatilization and chemical vapor deposition approach, we successfully developed N -doped carbon aerogels immobilized with separated iron sites (Fe-SAC@N/CA-Cd). The obtained Fe-SAC@N/CA-Cd exhibited substantially large specific surface area (S BET = 1173 m 2 /g) and a multi-level pore structure, which can effectively mitigate the random aggregation of Fe atoms during pyrolysis. As a result, it demonstrated appreciable activity and stability in catalyzing the ORR progress (E 1/2 = 0.88 V, E onset = 0.96 V). Furthermore, the assembled liquid electrolyte-state Zn-air batteries (LES-ZAB) and all-solid-state Zn-air battery (ASS-ZAB) also provides encouraging performance, with a peak power density of 169 mW cm −2 for LES-ZAB and a maximum power density of 124 mW cm −2 for ASS-ZAB.
研究领域:
材料科学
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电化学
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能源存储
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PubMed
高影响因子
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
·
2023
·Vol. 120
·期 14
·e2219043120
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IF 11.1
Huan Wang,Youzeng Li,Maoyu Wang,Shan Chen,Meng Yao,Jialei Chen,Xuelong Liao,Yiwen Zhang,Xuan Lu,Edward Matios,Jianmin Luo,Wei Zhang,Zhenxing Feng,Jichen Dong,Yunqi Liu,Weiyang Li
Despite the various strategies for achieving metal–nitrogen–carbon (M–N–C) single-atom catalysts (SACs) with different microenvironments for electrochemical carbon dioxide reduction reaction (CO2RR), the synthesis–structure–performance correlation remains elusive due to the lack of well-controlled synthetic approaches. Here, we employed Ni nanoparticles as starting materials for the direct synthesis of nickel (Ni) SACs in one spot through harvesting the interaction between metallic Ni and N atoms in the precursor during the chemical vapor deposition growth of hierarchical N-doped graphene fibers. By combining with first-principle calculations, we found that the Ni-N configuration is closely correlated to the N contents in the precursor, in which the acetonitrile with a high N/C ratio favors the formation of Ni-N3, while the pyridine with a low N/C ratio is more likely to promote the evolution of Ni-N2. Moreover, we revealed that the presence of N favors the formation of H-terminated edge of sp2 carbon and consequently leads to the formation of graphene fibers consisting of vertically stacked graphene flakes, instead of the traditional growth of carbon nanotubes on Ni nanoparticles. With a high capability in balancing the *COOH formation and *CO desorption, the as-prepared hierarchical N-doped graphene nanofibers with Ni-N3 sites exhibit a superior CO2RR performance compared to that with Ni-N2 and Ni-N4 ones.
研究领域:
材料科学
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电化学
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催化
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纳米技术
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高影响因子
Journal of Energy Chemistry
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2023
·
IF 13.1
Katam Srinivas,Zhuo Chen,Anran Chen,Fei Ma,Ming-qiang Zhu,Yuanfu Chen
The development of efficient single-atom catalysts (SACs) for the oxygen reduction reaction (ORR) remains a formidable challenge, primarily due to the symmetric charge distribution of metal single-atom sites (M-N 4 ). To address such issue, herein, Fe-N x sites coupled synergistic catalysts fabrication strategy is presented to break the uniform electronic distribution, thus enhancing the intrinsic catalytic activity. Precisely, atomically dispersed Fe-N x sites supported on N/S-doped mesoporous carbon (NSC) coupled with FeS@C core-shell nanoparticles (FAS-NSC@950) is synthesized by a facile hydrothermal reaction and subsequent pyrolysis. Due to the presence of an in situ-grown conductive graphitic layer (shell), the FeS nanoparticles (core) effectively adjust the electronic structure of single-atom Fe sites and facilitate the ORR kinetics via short/long-range coupling interactions. Consequently, FAS-NSC@950 displays a more positive half-wave potential ( E 1/2 ) of 0.871 V with a significantly boosted ORR kinetics (Tafel slope = 52.2 mV dec −1 ), outpacing the commercial Pt/C ( E 1/2 = 0.84 V and Tafel slope = 54.6 mV dec −1 ). As a bifunctional electrocatalyst, it displays a smaller bifunctional activity parameter (Δ E ) of 0.673 V, surpassing the Pt/C-RuO 2 combination (Δ E = 0.724 V). Besides, the FAS-NSC@950-based zinc-air battery (ZAB) displays superior power density, specific capacity, and long-term cycling performance to the Pt/C-Ir/C-based ZAB. This work significantly contributes to the field by offering a promising strategy to enhance the catalytic activity of SACs for ORR, with potential implications for energy conversion and storage technologies.
研究领域:
电化学
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材料科学
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能量转换与存储
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高影响因子
BIOSENSORS & BIOELECTRONICS
·
2022
·
IF 12.545
Nannan Wu,Hong Zhong,Yu Zhang,Xiaoqian Wei,Lei Jiao,Zhichao Wu,Jiajia Huang,Hengjia Wang,Scott P. Beckman,Wenling Gu,Chengzhou Zhu
Rational design and construction of electrochemical sensing platforms with high sensitivity and selectivity is one of the challenges in practical application. Although single-atom catalysts (SACs) have attracted extensive attention, atomically dispersed metal catalysts (ADCs) with multi-atom sites can further compensate for the deficiencies of SACs, which have gradually been a research hotspot in recent years. Herein, atomically dispersed Ru 3 site catalyst (Ru 3 /NC) is employed to catalyze small biomolecule oxidation , which exhibits much superior electrocatalytic ability of uric acid (UA) to Ru single-atom catalyst (Ru 1 /NC). What's more, theoretical calculations reveal that the enhanced performance is mainly derived from the dominant electronic structure of ADCs with multi-atom sites compared to SACs, leading to the more favorable adsorption of hydroxy anion groups, which can serve as one part of the active moiety and “promoter” to achieve the fast oxidation of small biomolecules. Our findings provide a new paradigm for designing promising catalysts to realize highly sensitive and selective small biomolecule detection and explore the catalytic mechanisms of small biomolecules at the atomic scale.
研究领域:
电化学
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催化
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材料科学
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分析化学
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生物分子传感
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DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）