ACS Catalysis
·
2022
·
IF 13.7
Wei Qu,Zhuoyun Tang,Hailin Wen,Manhui Luo,Tao Zhong,Qiyu Lian,Lingling Hu,Shuanghong Tian,Chun He,Dong Shu
High-performance and robust catalysts act as core drivers for catalytic ozonation to eliminate gaseous sulfur-containing volatile organic compounds (VOCs). Herein, nitrogen-doped carbon nanotubes embedded with Co species (Co@NCNT) are synthesized by thermolysis of a ZIF-67/melamine mixture. The carbon-confinement effects in Co@NCNT not only improve the stability of Co species but also regulate the electronic structure of Co─C bonds, consequently synergistically improving the catalytic ozonation performance. The experimental results indicate that the Co@NCNT catalyst could still remove ∼86% of odorous methyl mercaptan (CH3SH) after running for 60 h at 25 °C under an initial concentration of 50 ppm CH3SH and 40 ppm ozone, relative humidity of 60%, and space velocity of 600,000 mL h–1 g–1, outdistancing reported values under comparable reaction conditions. Detailed characterization and theoretical simulations reveal that the electronic metal–support interaction of Co─C bonds in Co@NCNT significantly adjusts the electronic structure of Co species, thereby promoting ozone-specific adsorption/activation to convert the surface atomic oxygen (*Oad) and ·OH/1O2/·O2–. Also, the electrons obtained from CH3SH in the electron-poor center transferred through the C─Co bond bridge to maintain the redox cycle of ≡Co0/2+ → ≡Co3+ → ≡Co0/2+ and realize the efficient and stable removal of CH3SH into CO2/SO42–/H2O. This work demonstrates that MOF-derived materials with tunable electronic structures achieve the stable removal efficiency for gaseous sulfur-containing VOCs via electron transfer trade-offs and provide potential candidate catalysts for the application of air purification.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Science China-Materials
·
2025
·
IF 7.4
Zhang Na,Xu Ziwei,Yang Zhou,Zhang Lu,Fan Zihao,Xu Dongfang,Wang Fei,Yuan Ningyi,Ding Jianning,Cui Jian,Liu Zhike
Inorganic perovskite solar cells (IPSCs) have garnered significant research interest in recent years owing to their excellent light and thermal stability, as well as their potential applications in tandem solar cells. However, the power conversion efficiency (PCE) and stability of IPSCs are often compromised by residual lattice stress and numerous defects at interfaces and within the bulk material, which lead to severe nonradiative recombination of photogenerated carriers. To address these challenges, we developed a zero-dimensional supramolecular complex, (ETP) 2 SbCl 5 , serving as both a dual interface and bulk modifier to regulate the growth of inorganic CsPbI 3 perovskite films. The (ETP) 2 SbCl 5 modifier exhibits a unique spatial distribution: the ETP + cations preferentially anchor at the buried interface, passivating defects on both TiO 2 and perovskite surfaces, while Sb 3+ and Cl − ions diffuse into the perovskite bulk during annealing, effectively relieving residual lattice stress. Moreover, Cl − anions accumulate on the top surface of the CsPbI 3 film, passivating cation defects. Consequently, the (ETP) 2 SbCl 5 -modified CsPbI 3 IPSC achieves a high-quality active layer with significantly reduced defects and suppressed energy loss, an impressive PCE of 21.71% and a high open circuit voltage of 1.27 V, remaining 97.4% of their initial efficiency after 500 h of continuous maximum power point (MPP) tracking.
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DOI
高影响因子
EcoMat
·
2024
·Vol. 6
·期 12
·e12501
·
IF 10.7
Zhongqi Xie,Huiming Luo,Qing-Song Jiang,Ya Zhao,Yong Peng,Ligang Yuan,Keyou Yan,Mojtaba Abdi-Jalebi
Two-dimensional Ruddlesden-Popper (2D RP) layered metal-halide perovskites have garnered increasing attention due to their favorable optoelectronic properties and enhanced stability in comparison to their three-dimensional counterparts. Nevertheless, precise control over the crystal orientation of 2D RP perovskite films remains challenging, primarily due to the intricacies associated with the solvent evaporation process. In this study, we introduce a novel approach known as reverse-cool annealing (RCA) for the fabrication of 2D RP perovskite films. This method involves a sequential annealing process at high and low temperatures for wet perovskite films. The resulting RCA-based perovskite films show the smallest root-mean-square value of 23.1 nm, indicating a minimal surface roughness and a notably compact and smooth surface morphology. The low defect density in these 2D RP perovskite films with exceptional crystallinity suppresses non-radiative recombination, leading to a minimal non-radiative open-circuit voltage loss of 149 mV. Moreover, the average charge lifetime in these films is extended to 56.3 ns, thanks to their preferential growth along the out-of-plane direction. Consequently, the leading 2D RP perovskite solar cell achieves an impressive power conversion efficiency of 17.8% and an open-circuit voltage of 1.21 V. Additionally, the stability of the 2D RP perovskite solar cell, even without encapsulation, exhibits substantial improvement, retaining 97.4% of its initial efficiency after 1000 hours under a nitrogen environment. The RCA strategy presents a promising avenue for advancing the commercial prospects of 2D RP perovskite solar cells.
研究领域:
材料科学
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能源技术
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纳米技术
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固体物理学
✓ 已验证
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2024
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IF 7.4
Xiaodong Chen,Jing Liao,Ke Yin,Lu Cheng,Zhewen Yang,Zewei Liu,Bichun Huang
Carbon materials derived from single biomass feedstock typically have serious defects such as low porosity and poor distribution of functional groups. In this work, a series of porous carbons with different mass ratios of porphyra and corn stalk (7:3, 1:1, and 3:7) were prepared by ingeniously utilizing co-pyrolysis coupled with KOH activation. The prepared porous carbon samples were characterized by N 2 adsorption/desorption isotherms, Field emission scanning electron microscopy, Transmission electron microscopy, X-ray diffraction, Raman spectroscopy, Elemental analysis, Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, and Thermo-gravimetric analysis. Results showed that the prepared CPPC73 possessed excellent adsorbent properties, including high specific surface area (2719 m 2 /g), large pore volume (1.225 cm 3 /g), hierarchical porous structure, and optimal distribution of N-containing functional groups. Chlorobenzene (CB) dynamic adsorption experiments indicated that CPPC73 had higher adsorption performance (1134 mg/g) than unmodified POPC (795 mg/g). A combination of density functional theory (DFT) calculations, correlation analysis, and Grand canonical Monte Carlo (GCMC) calculations was performed to clarify the CB adsorption mechanism. Correlation analysis and GCMC calculations confirmed that pores in the range of 0.7–2.0 nm were the best adsorption sites for CB. Furthermore, DFT calculations indicated that N/O-containing functional groups on the carbon surface enhanced the interaction between porous carbon and CB, especially the pyrrolic-N. This work offers a new strategy to convert waste seaweed into a high-performance adsorbent for Cl-VOCs removal.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2023
·
IF 11.4
Boge Zhang,Yongjie Shen,Biyuan Liu,Jian Ji,Wenjing Dai,Pingli Huang,Dengsong Zhang,Guangqin Li,Ruijie Xie,Haibao Huang
Ozone catalytic oxidation (OZCO) has gained great interest in environmental remediation while it still faces a big challenge during the deep degradation of refractory volatile organic compounds (VOCs) at room temperature. Hydroxylation of the catalytic surface provides a new strategy for regulating the catalytic activity to boost VOC degradation. Herein, OZCO of toluene at room temperature over hydroxyl-mediated MnOx/Al2O3 catalysts was originally demonstrated. Specifically, a novel hydroxyl-mediated MnOx/Al2O3 catalyst was developed via the in situ AlOOH reconstruction method and used for toluene OZCO. The toluene degradation performance of MnOx/Al2O3 was significantly superior to those of most of the state-of-the-art catalysts, and 100% toluene was removed with an excellent mineralization rate (82.3%) and catalytic stability during OZCO. ESR and in situ DRIFTs results demonstrated that surface hydroxyl groups (HGs) greatly improved the reactive oxygen species generation, thus dramatically accelerating the benzene ring breakage and deep mineralization. Furthermore, HGs provided anchoring sites for uniformly dispersing MnOx and greatly enhanced toluene adsorption and ozone activation. This work paves a way for deep decomposition of aromatic VOCs at room temperature.
研究领域:
环境科学
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催化
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化学工程
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大气化学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Jinxi Feng,Tiantian Zhang,Wen Yan,Jingxiang Sun,Shuanghong Tian,Zhili He,Ya Xiong
A new piezo-catalytic reactor (PCR) was constructed. It was used to investigate the piezocatalytic degradation of pollutants and simultaneous response of current. It was found that PCR with SnO 2 / t -BaTiO 3 /ITO film anode possessed a more favourable piezocatalytic degradation and piezo-current response than PCR with only ITO or t -BaTiO 3 /ITO film anode, individually. For HCOOH, the degradation rate, short circuit current (I sc ) and open-circuit voltage (V oc ) reached 77.8 mg·L -1 ·h −1 , 5.12 µA, and 0.65 V, respectively, under its optimal condition. Its anodic process predominantly involved the piezocatalytic oxidations of H 2 O to •OH and HCOOH to CO 2 , while the cathodic process was mainly related to the reduction of O 2 to •O 2 – or H 2 O 2 and reduction of H + ion to H 2 . Although these processes were depended on the energy band structure of t -BaTiO 3 and redox potential of cathodic reactions, they were all initiated by the piezoelectric effect of t -BaTiO 3 , which drove the separation of intrinsic free carries to generate oxidative holes and reductive electrons. These investigation results and findings not only deepened the understanding of its piezo-current response, but also possibly extended the application of piezocatalysis to fuel cell.
研究领域:
环境科学
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材料科学
·
催化
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
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