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ACS Applied Energy Materials · 2021 · IF 6.024

Reaction Mechanism of the Enhanced Reaction Activity and Rate of N-Doped CoO Photocatalysts for Photoreduction of CO2 in Air

Jingjing Wu,Jie Chen,Jingxuan Hao,Baoxin Ni,Dong Yang,Sheng Zhu,Qunjie Xu,Yulin Min

The use of light to directly reduce CO2 in the atmosphere is the actual development trend of photocatalysis applications in the future. However, it is still in the initial stage of exploration. In this work, oleylamine is used as a template in a one-step hydrothermal method to obtain the N-doped CoO catalyst that can be used to efficiently reduce CO2 in air. N-doped CoO achieves ultrahigh CO2 conversion efficiency (about 75%), amazing CO yield (2.902 mmol g–1 h–1), and superior CO conversion frequency (TOFCO > 300) in air. However, in a 0.03% simulated atmosphere (Ar/CO2), the CO precipitation rate drops by 18 times, while the H2 precipitation rate increases significantly. Quasi-in situ spectroscopy and experimental studies show that O2 in the CO2 reduction process will promote the formation of an amorphous layer with a small number of hydroxyl groups on the surface of N-doped CoO. This amorphous/crystalline interface will effectively promote the catalytic reduction of CO2. This work has inspired further research on the photoreduction process of low-concentration CO2 in the future.

CAS / MDL: 112-90-3 144-55-8
研究领域: 材料科学 · 环境科学 · 光催化技术
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JOURNAL OF ALLOYS AND COMPOUNDS · 2018 · IF 3.779

The formation and evolution mechanism of amorphous layer surrounding Nb nano-grains in Nb-Al system during mechanical alloying process

Xinhua Li,Xin Wen,Huanhuan Zhao,Zongqing Ma,Liming Yu,Chong Li,Chenxi Liu,Qianying Guo,Yongchang Liu

The microstructure and phase evolution in Nb-Al system during MA are systemically studied. The existence of Nb-Al amorphous layer surrounding Nb nano-grains after short-time ball milling was confirmed by the HRTEM observation as well as the crystallization behavior in the annealing experiment. It was also found that after short time milling, only very little Al can enter the crystal lattice of Nb and substitute for Nb, whereas most of Al mainly concentrate in this amorphous layer surrounding Nb nano-grains. What's more, interface thermodynamic analysis and calculation were employed to investigate the phase formation and evolution of this amorphous layer in Nb-Al binary system during MA process. Accordingly, positive driving force (≡-ΔG) definitely exists for the formation of the amorphous layer {NbAl} surrounding Nb nano-grains. Thus, these amorphous layers can form and exist stably in the short-time milled Nb-Al system. With the milling time prolonging, this amorphous layer becomes unstable and can crystallize into Nb(Al) ss solid solution when its thickness increases beyond a critical thickness. The critical thickness of this amorphous layer is also predicted by the interface thermodynamics calculation and the corresponding calculated value (approximately 1.9 nm) is consistent with the observed thickness (about 2.2 nm) by the HRTEM within the error range. More importantly, the solubility of Al in the lattice of Nb can be significantly increased resulting from the crystallization of this amorphous layer {NbAl}. Our work provides a new and rational perspective to well understand the complicated microstructure and phase evolution in various nano-sized systems during MA process.

CAS / MDL: 7440-03-1 7429-90-5
研究领域: 材料科学 · 物理冶金学
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APPLIED SURFACE SCIENCE · 2024 · IF 6.3

Interface oxidation induced amorphous/crystalline 1D hollandite Rb0.17IrO2 for efficient oxygen evolution reaction

Dan-Ni Li,An-hui Zhou,Xiang Shao,Lin Zhu,Yan Du,Li-Mei Cao,Cheng-Long Ma,Ji Yang

Recently, surface reconstruction derived from Ir-based derivatives could achieve satisfactory oxygen evolution performance. Herein, ultra-long nanowire hollandite structured Rb 0.17 IrO 2 was synthesized and a nano-amorphous layer with a thickness of ∼1.5 nm was achieved by interfacial oxidation treatment. The prepared catalyst exhibits outstanding water oxidation activity with an oxygen evolution reaction (OER) current density of 10 mA cm −2 at 330 mV for robust continuous operation in acidic media. Through the spectroscopic and density functional theory (DFT) theoretical calculations, we demonstrate that the nano-amorphous layers induced by interfacial oxidation on the one-dimensional (1D)-nanowire surface have enhanced O-2p centers and increased Ir-O hybridization compared to the bulk Rb 0.17 IrO 2 phase, which essentially balances the adsorption energy of the intermediates. Effectively incorporating surface reconstruction behavior could significantly improve catalyst activity. This work effectively combines 1D Ir-based materials and surface reconstruction, which provides a strategy for the subsequent full utilization of Ir-based materials applied on OER process.

CAS / MDL: 14996-61-3 31175-20-9
研究领域: 材料科学 · 电化学
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CHINESE JOURNAL OF CHEMICAL ENGINEERING · 2019 · IF 1.911

Engineering an ultrathin amorphous TiO2 layer for boosting the weatherability of TiO2 pigment with high lightening power

Yangyang Yu,Kejing Wu,Shiyu Lu,Kui Ma,Shan Zhong,Hegui Zhang,Yingming Zhu,Jing Guo,Hairong Yue,Changjun Liu,Siyang Tang,Bin Liang

TiO 2 pigments are typically coated with inert layers to suppress the photocatalytic activity and improve the weatherability. However, the traditional inert layers have a lower refractive index compared to TiO 2 , and therefore reduce the lightening power of TiO 2 . In the present work, a uniform, amorphous, 2.9-nm-thick TiO 2 protective layer was deposited onto the surface of anatase TiO 2 pigments according to pulsed chemical vapor deposition at room temperature, with TiCl 4 as titanium precursor. Amorphous TiO 2 coating layers exhibited poor photocatalytic activity, leading to a boosted weatherability. Similarly, this coating method is also effective for TiO 2 coating with amorphous SiO 2 and SnO 2 layers. However, the lightening power of amorphous TiO 2 layer is higher than those of amorphous SiO 2 and SnO 2 layers. According to the measurements of photoluminescence lifetime, surface photocurrent density, charge-transfer resistance, and electron spin resonance spectroscopy, it is revealed that the amorphous layer can prevent the migration of photogenerated electrons and holes onto the surface, decreasing the densities of surface electron and hole, and thereby suppress the photocatalytic activity.

研究领域: 材料科学 · 化学工程
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CERAMICS INTERNATIONAL · 2022 · IF 5.532

Alpha-particle irradiation effects of Nd-doped Y3Fe5O12 ceramics

Kexin Lv,Hengcheng Wan,Yi Li,Shengtai Zhang,Qiang He

The garnet structure Y 3 Fe 5 O 12 (YIG) possesses a high immobilization capacity for actinides. However, the related research on the sensitivity of garnet structures to irradiation damage is still in its infancy. Herein, we synthesize Y 3-x Nd x Fe 5 O 12 (x = 0.1, 1.8) ceramics and irradiate them with 2 MeV α-particle irradiation to fluences ranging from 1 × 10 14 to 1 × 10 17 ions/cm 2 at room temperature. We evaluated the effects of irradiation damage on the phase transition and chemical stability. An amorphous layer with a thickness of 84 nm is formed by irradiation, though the grain shape and element distribution remain uniform after irradiation. In addition, Y 3-x Nd x Fe 5 O 12 (x = 0.1, 1.8) ceramics exhibit excellent chemical stability (∼ 10 −5  g m −2 · d −1 ) in the leaching process. Restricted by the topological structure of garnet, the increase in solid solubility does not lead to a change in the radiation tolerance of the garnet structure, which means that garnet of different compositions should have similar and predictable radiation tolerance.

研究领域: 材料科学 · 核科学 · 固体物理
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Materials Today Chemistry · 2024 · IF 6.7

A novel strategy for design of mechanically robust antifouling coatings via bifunctional domain engineering

Peng-Yu Zhu,Tian-Xiao Liang,Muhammad Arslan Hafeez,Muhammad Yasir,Dan-Qing Feng,Chun-Feng Ma,Cheng Zhang,Lin Liu

The issue of biofouling on marine structures carries significant economic and ecological implications, necessitating the development of effective and durable antifouling coatings. Traditional organic antifouling coatings often struggle with mechanical robustness in harsh marine environments, making them fragile and highly susceptible to abrasion. To address these challenges, we propose a novel “bifunctional domain engineering” strategy for designing robust antifouling coatings that combines excellent mechanical strength of a Fe-based amorphous layer and high antifouling efficacy of an incorporated organics. The hard domains consist of Fe-based amorphous micro humps, providing a sturdy framework that enhances the coating's mechanical durability. In contrast, the soft domains comprise epoxy resin infused with Cu 2 O and 4,5-Dichloro-2- n -octyl-4-isothiazolin-3-one (DCOIT), offering a dual-action antifouling function via controllable antifouling agent release. Evaluation of antifouling performance by lab tests against Pseudomonas aeruginosa , Staphylococcus aureus , and Chlorella algae and practical marine field tests (for 150 days) demonstrates significant reductions in bacterial and algal adhesion (nearly 100 % resistance) with the bifunctional domain engineered coating (referred to as HSR coating), compared to pure amorphous coating . Mechanical durability tests, including abrasion and erosion experiments, underscore the HSR coating's excellent wear resistance. Importantly, the HSR coating maintains its outstanding antifouling properties even after 1000 abrasion cycles, highlighting its potential for long-term marine applications in harsh conditions. This study lays the groundwork for design of robust antifouling coatings capable of withstanding the harsh operating environments while effectively combating biofouling.

CAS / MDL: 64359-81-5
研究领域: 材料科学 · 海洋生物学 · 生物医学工程
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ELECTROCHIMICA ACTA · 2020 · IF 6.215

Mechanism on BiVO4 photoanode photoelectrochemical performance improving: Based on surface electrochemical reduction method

Yaping Zhang,Yuyu Bu,Fengqiu Jiang,Huan Li,Xi Chen,Jin-Ping Ao

In this work, a typical BiVO 4 photoanode is employed to explore the performance improving mechanism by surface electrochemical reduction. Corresponding results demonstrate some new information that nanoparticle-like amorphous layer is formed on the surface of BiVO 4 and its thickness is positive correlation with the SER force. Furthermore, Scanning Kelvin probe results indicate that the Fermi level of the amorphous layer is shifted positively, inducing a homojunction built-in electric field between the amorphous layer and the bulk BiVO 4 . The transfer ability of photogenerated holes from the bulk to the surface of photoanode can enhance obviously. In addition, due to the quasi-oxygen vacancy defects in the amorphous layer, the enhanced hydrophilicity improves the PEC performance synergistically. However, as the thickness of amorphous layer increasing, it raises the migration time and secondary recombination rate of the photogenerated carriers. Therefore, a controllable amorphous surface and PEC performance of BiVO 4 photoanode can realize by adjusting the SER force.

研究领域: 材料科学 · 电化学
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Journal of Materials Chemistry A · 2021 ·Vol. 10 ·期 3 ·1369-1379 · IF 12.732

In situ surface reconstruction of a Ni-based perovskite hydroxide catalyst for an efficient oxygen evolution reaction

Yegui Fang,Yusheng Fang,Ruoqi Zong,Zhouyang Yu,Youkun Tao,Jing Shao

One core reaction involved in many electrochemical energy conversion systems is the oxygen evolution reaction (OER), which usually dominates the overall polarization loss due to its sluggish kinetics. Activating O2 electrocatalysis on the catalyst surface requires effective regulation of the surface spatial and electronic structure to facilitate the in situ generation of active species. Here, we report an in situ surface reconstruction method to boost the activity of a Ni-based perovskite hydroxide, NiSn(OH)6, for OER catalysis. The surface reconstruction is modulated by anodic polarization during the OER process, building a Ni3+-containing amorphous layer with selective Sn etching. Taking advantage of the in situ surface amorphization that facilitates the generation of active metal oxy(hydroxide) species, a significant performance enhancement is achieved on NiSn(OH)6. Theoretical calculations further demonstrate that the Sn vacancies on the surface optimize the electronic structure of the Ni sites and promote the adsorption of the reaction intermediates.

研究领域: 电化学 · 催化 · 材料科学 · 表面科学
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