Environmental Science-Nano
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2024
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IF 5.8
Shengnan Zhang,Lingyi Li,Junxue Li,Wei Cheng
Hematite displays diverse crystal structures and often coexists with Fe(II), both of which are crucial in controlling the fate and mobility of Cr(VI). However, the mechanisms underlying Cr(VI) removal in the presence of Fe(II) on various hematite facets remain elusive. This study aims to elucidate the facet-dependent reactivity of hematite nanocrystals in conjunction with Fe(II) for the removal of Cr(VI) from aqueous solutions. Hematite nanoplates (HNPs), predominantly composed of {001} facets, and nanorods (HNRs), exposing both {001} and {110} facets, were synthesized and characterized. Their Cr(VI) removal capabilities were evaluated in hematite–Cr(VI) and hematite–Fe(II)–Cr(VI) systems, as well as the Fe(II)–Cr(VI) system. The adsorption of Fe(II) and Cr(VI) on hematite surfaces was highly dependent on the crystal facets and pH, with HNRs demonstrating superior Cr(VI) adsorption over HNPs, especially under acidic conditions. Neutral pH favored Fe(II)–Cr(VI) redox reactions and Fe(II) adsorption. The hematite–Fe(II) couple displayed a synergistic effect in removing Cr(VI) under acidic conditions, which was not observed under neutral conditions. The presence of Fe(II) notably enhanced Cr(VI) adsorption onto hematite, and bound Fe(II) facilitated electron transfer, accelerating Cr(VI) reduction. HNRs–Fe(II) exhibited higher Cr(VI) removal efficiency than HNPs–Fe(II) due to their lower free corrosion potential and improved electron transport properties. This research underscores the potential of facet engineering in optimizing hematite nanocrystals for environmental remediation, specifically in Cr(VI)-contaminated environments.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Sufang Yang,Xiaobo Yang,Qiang Wang,Xueqin Cui,Houbing Zou,Xili Tong,Nianjun Yang
Surface atomic structures of transition metal phosphides determine the electrocatalytic activities toward hydrogen evolution reaction (HER). In this work, we developed a new facet-guided phosphorization strategy to synthesize Rh 2 P electrocatalysts with tunable facet exposure and further unveil their intrinsic facet-dependent HER activity in pH-universal media. The Rh 2 P nanoparticles feature {1 1 1} and {2 0 0} facets when the precursors of Rh nanoctahedron and nanocube are used, respectively. The Rh 2 P{2 0 0} catalyst showed a remarkable HER performance with the overpotential of 23, 22 and 54 mV at a current density of 10 mA cm −2 in 1.0 M KOH, 0.5 M H 2 SO 4 and 1.0 M phosphate buffer, respectively. The mass activity and specific activity of Rh 2 P{2 0 0} were 3~5-times higher than those of Rh 2 P{1 1 1} and Pt/C catalysts. As elucidated using theoretical calculations, the overlapping of Rh-4d and P-3p of Rh 2 P{2 0 0} and Rh 2 P{1 1 1} results in distinct electronic states of surface Rh atoms, leading to varied free energies for water dissociation and hydrogen adsorption/desorption.
研究领域:
材料科学
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电化学
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催化科学
✓ 已验证
DOI
高影响因子
ACS Applied Optical Materials
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2025
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IF 3.8
Yan Zhang,Junzhe Wang,Liang Li,Honggang Zhang,Bei Li,Xiangxiang Zhang,Zeyan Wang,Yuanyuan Liu,Peng Wang,Hefeng Cheng,Ying Dai,Baibiao Huang,Zhaoke Zheng
The design of organic–inorganic heterojunctions can facilitate the separation of photoinduced charge carriers by modulating the electronic structure at the surface and interface states, showing promising applications in the field of photocatalytic CO2 cycloaddition. However, the details of the surface/interface effects between these two components are still poorly understood. Herein, Cu2O@Cu3(HHTP)2 (HHTP = 2, 3, 6, 7, 10, 11-hexahydroxytriphenylene) heterojunctions were synthesized, where Cu2O nanoparticles (NPs) featuring distinct crystal facets were utilized as substrates for the in situ growth of the copper-based metal–organic framework (Cu3(HHTP)2). Among them, t-Cu2O@Cu3(HHTP)2, centered on t-Cu2O with {111} and {100} facets, exhibits superior performance toward photocatalytic CO2 cycloaddition to chlorinated propylene carbonate, with a conversion efficiency of 372 mmol g–1 h–1 under light. Notably, single-particle spectroscopy reveals a more efficient photogenerated carrier transfer between t-Cu2O and Cu3(HHTP)2. The results confirm that crystalline facet dependence is a key factor in semiconductor photocatalysis and an important strategy for optimizing the reactivity of photocatalysts, which provides a way to improve the photocatalytic CO2 cycloaddition performance by modulating the interfacial states of organic–inorganic heterojunction structures.
研究领域:
材料科学
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催化化学
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物理化学
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产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
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2024
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IF 6.5
Hao Yan,Mingyue Zhao,Yueqiang Cao,Xin Zhou,Yibin Liu,Xiaobo Chen,Xiang Feng,Xuezhi Duan,Francisco Zaera,Xinggui Zhou,Chaohe Yang
In-depth understanding and precise tuning of the crystal facet-dependent catalytic properties of supported catalysts are critical for polyol oxidation. Herein, we report a crystal-facet-dependent study of Au-ZnO interfaces for the selective promotion of the oxidation of various polyols and alcohols (glycerol, 1,2-propanediol, 1,2-butanediol, and isopropanol) at the secondary hydroxyl position to produce the corresponding ketones. Three facets of the zinc oxide support, ZnO(1 0 1), ZnO(1 0 0) and ZnO(0 0 1), associated with nanoparticles of various morphologies (spherical (S), rod (R) and disk (D), respectively), were found to induce different electronic local environments and surface oxygen vacancy contents at the Au-ZnO interface. In particular, the ZnO(0 0 1) facet dominating in the Au/ZnO-D nanoparticles can store more electrons from Au, and such electron sink effect, together with the generation of oxygen vacancies (Zn-O v ), synergistically enhances the adsorption of O 2 and polyols at the secondary hydroxyl position. Moreover, it was determined that the as-formed Au δ+ -OH* site resulting from O 2 activation can efficiently extract the hydrogen of the C-H bond of the key RCHO*CH 2 OH intermediate on the Zn-O v site of ZnO(0 0 1) surfaces. Consequently, the Au/ZnO-D catalyst exhibits unprecedented catalytic activity (turnover frequency >500 h −1 ) and ketone selectivity (>80 %) for glycerol oxidation.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2024
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IF 12.2
Dan Su,Xiaoyan He,Jiangwei Zhou,Chengqing Yuan,Xiuqin Bai
Biofilms adhering to different surfaces have significant negative impacts in various fields. Cerium oxide nanoparticles can serve as mimics of haloperoxidase for biological biofilm inhibition applications. The regulation of the exposed facet of CeO 2 nanoparticles influences their efficiency in various catalytic processes. However, there is still a lack of systematic studies on the facet-dependent haloperoxidase-like activity of CeO 2 . In the present study, the facet-dependent haloperoxidase activities and antibiofilm performance of CeO 2 nanoparticles were elucidated through experiment analysis and density function theory calculation. The as-prepared CeO 2 nanoparticles inhibited bacterial survival and catalyzed the oxidative bromination of quorum sensing signaling molecules, achieving biofilm inhibition performance. The antibacterial and biofilm formation suppression abilities were consistent with their haloperoxidase activities. The {111}- and {110}-facet CeO 2 nanopolyhedra, as well as the {110}- and {100}-facet CeO 2 nanorods , which had higher haloperoxidase activity showed better antibiofilm performance than the {100}-facet CeO 2 cubes. The present findings provide a comprehensive understanding of the facet-dependent haloperoxidase-like activity of CeO 2 . Furthermore, engineering CeO 2 morphologies with different crystal facets may represent a novel method for significantly adjusting their haloperoxidase-like activity.
研究领域:
材料科学
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微生物学
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催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Tong Li,Ze-Zhou Ding,Fei Shi,Yi-Ting Ju,Ting-Ting Du,Chang Liu,Xing Zhang
CuO is currently used as an effective activator for peroxymonosulfate (PMS), which exhibits complex radical, nonradical, or both activation pathways. However, there exists a knowledge gap concerning the relationship between CuO exposed facets and the PMS activation pathway, which should require further investigation. This study employed a simple and facile hydrothermal method to controllably prepare CuO samples with exposed {010} and {001} facets (referred to as CuO-010 and CuO-001, respectively). The main aim was to further study the facet-dependent PMS activation mechanism. The experimental results showed that the CuO-001 exhibited significantly higher activation efficiency than the CuO-010 due to the different surface atomic arrangement. Furthermore, scavenging experiments and EPR analyses revealed that CuO-010 exhibited both radical ( SO 4 • − and •OH) and non-radical ( 1 O 2 ) pathways, synergistically degraded tetracycline (TC) and 4-nitrophenol (4-NP). Conversely, the CuO-001 displayed non-radical ( 1 O 2 ) and Cu(Ⅲ) intermediates, collaborating to oxidize the degradation of TC and 4-NP. More importantly, the generated 1 O 2 species and Cu(Ⅲ) intermediates exhibited a preference for reacting with amino or phenolic compounds containing electron-rich functional groups. Moreover, the CuO-001 also showed excellent resistance to anion interference, stability, and compatibility of a wide pH range. The outcomes of this study provide new insights into the comprehensiveness facet-dependent activation of PMS and the design of efficient metal oxide catalysts using the facet strategy for effective degradation of amino/phenolic pollutants in wastewater.
研究领域:
环境科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子