Nature Communications
·
2025
·Vol. 16
·期 1
·1-12
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IF 15.7
Wang Jian,Zhang Jiahe,Li Yang,Xia Xinghui,Yang Hengjing,Kim Jae-Hong,Zhang Wen
Photocatalytic water disinfection technology is highly promising in off-grid areas due to abundant year-round solar irradiance. However, the practical use of powdered photocatalysts is impeded by limited recovery and inefficient inactivation of stress-resistant bacteria in oligotrophic surface water. Here we prepare a floatable monolithic photocatalyst with ZIF-8-NH 2 loaded Ag single atoms and nanoparticles (Ag SA+NP /ZIF). Atomically dispersed Ag sites form an Ag−N charge bridge, extending the lifetime of charge carriers and thereby promoting reactive oxygen species (ROS) generation. The photothermal effect of the plasmonic Ag nanoparticles reduces the bacterial resistance to ROS and impairs DNA repair capabilities. Under sunlight irradiation, the synergistic effect of Ag single atoms and nanoparticles enables 4.0 cm 2 Ag SA+NP /ZIF to achieve over 6.0 log inactivation (99.9999%) for the stress-resistant Escherichia coli ( E. coli ) in oligotrophic surface water within 30 min. Furthermore, 36 cm 2 Ag SA+NP /ZIF is capable of disinfecting at least 10.0 L of surface water, which meets the World Health Organization (WHO) recommended daily per capita drinking water allocation (8.0 L). This study presents a decentralized and sustainable approach for water disinfection in off-grid areas.
研究领域:
环境科学
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材料科学
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微生物学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Haiqiang Mu,Yu-An Li,Xiuli Wang,Feng Li,Xin Du,Jing Li
The rational modulation of the coordination environment of the active center of single-atom catalysts (SACs) is a potential strategy to improve the activity and selectivity of electrocatalytic CO 2 reduction. We developed a series of single-atom Ag-anchored on N -doped carbon catalysts with different N -coordination environments by regulating the carbon source (glucose/graphene oxide, GO). Results demonstrated that the CO 2 -to-CO/C 2 H 5 OH pathway can be converted through reasonable regulation of the content of pyrrolic N and pyridine N. At a highly dominant pyrrolic N content of 40.0 %, the electrocatalyst of Ag-N-rGO 0.025 M facilitates the formation of CO with a Faradaic efficiency (FE) of 69.7 %. By contrast, when the pyridine N content is 70.5 %, the best Ag-N-C 0.05 M catalyst in the H-cell shows an FE of 42 % for C 2 H 5 OH at −0.97 V vs. RHE; moreover, the FE is stable at 40 % within 31 h. Density functional theory calculations further confirm that the pyrrolic N site is conducive to the conversion of CO 2 to intermediate *CO, whereas pyridine N exhibits the highest binding energy (ΔG = -4.73 eV) to hold *CO intermediates for dimerization, consequently steering the pathway to the formation of C 2 H 5 OH. The results of this study provide novel insights into the rational design of carbon-based SACs based on efficient electrochemical CO 2 reduction reaction and the regulation of CO 2 selectivity and activity for C 2 H 5 OH production.
研究领域:
材料科学
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电化学
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催化反应
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产品关联
DOI
高影响因子
Small
·
2023
·Vol. 19
·期 34
·2301610
·
IF 13.3
Wenjun He,Rui Zhang,Hui Liu,Qiuyan Hao,Ying Li,Xuerong Zheng,Caichi Liu,Jun Zhang,Huolin L. Xin
Bimetallic layered double hydroxides (LDHs) are promising catalysts for anodic oxygen evolution reaction (OER) in alkaline media. Despite good stability, NiCo LDH displays an unsatisfactory OER activity relative to the most robust NiFe LDH and CoFe LDH. Herein, a novel NiCo LDH electrocatalyst modified with single-atom silver grown on carbon cloth (Ag SA -NiCo LDH/CC) that exhibits exceptional OER activity and stability in 1.0 m KOH is reported. The Ag SA -NiCo LDH/CC catalyst only requires a low overpotential of 192 mV to reach a current density of 10 mA cm −2 , obviously boosting the OER activity of NiCo LDH/CC (410 mV@10 mA cm −2 ). Inspiringly, Ag SA -NiCo LDH/CC can maintain its high activity for up to 500 h at a large current density of 100 mA cm −2 , exceeding most single-atom OER catalysts. In situ Raman spectroscopy studies uncover that the in situ formed NiCoOOH during OER is the real active species. Hard X-ray absorption spectrum (XAS) and density functional theory (DFT) calculations validate that single-atom Ag occupying Ni site increases the chemical valence of Ni elements, and then weakens the adsorption of oxygen-contained intermediates on Ni sites, fundamentally accounting for the enhanced OER performance.
研究领域:
材料科学
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催化化学
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能源化学
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产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Teng Zhang,Xingyu Lu,Wei Qi,Gaowu Qin,Song Li
The electrochemical reduction of CO 2 to CO is considered to be one of the most mature routes that could be commercialized for efficient utilization of large amount of CO 2 . Silver (Ag) has shown high selectivity towards CO but usually requires high reduction potential. Herein, a novel Ag single atom-polyaniline (PANI) is constructed directly on gas diffusion electrode (GDE). The amino group with strong electron-donating ability in PANI can effectively promote the adsorption and activation of CO 2 . In addition, the adsorption of *COOH is significantly enhanced on N-coordinated Ag. The proposed catalyst electrode shows an outstanding performance with the Faraday efficiency of CO close to 100% at −0.75 V (vs. RHE), the energy efficiency is 12.8% and the output of CO is 108.7 mL cm −2 h −1 , which exceeds most state-in-art Ag-based catalysts, highlighting the importance for the rational design and controllable fabrication of active sites and their favorable chemical environments.
研究领域:
材料科学
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环境科学
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电化学
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Lin Jin,Yajuan Wei,Lanlan Feng,Yuwen Wang,Shuang Liu,Junwei Zhang,Ruoxuan Ma,Xueying Shao,Xuan Zhang,Demeng Kong,Zibo Zhao,Wei Zhang,Jia Liu,Jingbo Zhang
The construction of ultra-close 2D atomic-thickness Van der Waals heterojunctions with high-speed charge transfer still faces challenges. Here, we synthesized single-layer ZnIn 2 S 4 and g-C 3 N 4 , and introduced silver single atoms to regulate Van der Waals heterojunctions at the atomic level to optimize charge transfer and catalytic activity. At the atomic scale, the impact of detailed structural differences between the two characteristic surfaces of ZnIn 2 S 4 ([Zn-S 4 ] and [In-S 4 ]) on catalytic performance has been first proposed. Experiments combined with the DFT study demonstrate that single atom Ag not only acts as a charge transfer bridge but also regulates the energy band and intrinsic catalytic activity. Benefiting from the enhanced electron delocalization, the synthesized catalyst ZIS/Ag@CN exhibits excellent photocatalytic performance, with a hydrogen production rate of 5.50 mmol·g −1 ·h −1 , which is much higher than the reported Ag-based single-atom catalysts so far. This work provides a new understanding of atomic-level heterojunction interface regulation and modification.
研究领域:
材料科学
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化学
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催化
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纳米技术
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能源材料
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）