CHINESE JOURNAL OF STRUCTURAL CHEMISTRY
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2024
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IF 5.9
Maomao Liu,Guizeng Liang,Ningce Zhang,Tao Li,Lipeng Diao,Ping Lu,Xiaoliang Zhao,Daohao Li,Dongjiang Yang
Rationally constructed new catalyst can promote carbon dioxide reduction reaction (CO 2 RR) to valuable carbonaceous fuels such as formate and CO, providing a promising strategy for low CO 2 emissions. Herein, the synthesized Ni 3 S 2 @C as a highly efficient electro-catalyst exhibits remarkable selectivity for formate with 73.9% faradaic efficiency (FE) at −0.7 V vs. RHE. At high applied potential, it shows a high syngas evolution with CO/H 2 ratios (0.54–3.15) that are suitable for typical downstream thermochemical reactions . The experimental and theoretical analyses demonstrate that the electron-rich Ni 2+ in Ni 3 S 2 enhances the adsorption behavior of ∗ OCHO intermediate, reduces the energy barrier of the formation of intermediates, and improves the selectivity of the formate product. Attenuated total reflection surface-enhanced infrared absorption spectra conducted in situ show that ∗ OCHO intermediate is more likely to be generated and adsorbed on Ni 3 S 2 , enhancing the selectivity and activity of the formate product.
研究领域:
电化学
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催化材料
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可再生能源
✓ 已验证
产品关联
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
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2022
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IF 5.876
Cheng Yan,Yue Wu,Haifeng Lu,Hailong Liu,Gang Yi,Mei Li,Xiaoxia Cai,Sheng Gao,Zhizhou Yang
Novel phenothiazine-based hyper-cross-linked porous polymers (PZ-HCPs) containing N, S double electron-rich atoms were synthesized using Friedel-Crafts alkylation reaction. Nitrogen adsorption-desorption test showed that the specific surface areas (S BET ) of the PZ-HCPs were between 131 m 2 g −1 and 209 m 2 g −1 . In addition, the π-electron-conjugated structure and the presence of N and S electron-rich heteroatoms in the PZ-HCPs facilitated its high iodine capture ability in both iodine solution and iodine vapor. Meanwhile, adsorption mechanism studies showed that the adsorbed iodine in the adsorbent existed as I 3 – and I 5 – . The adsorption behavior of PZ-HCP-1:4 for iodine conformed to the pseudo-second-order (PSO) kinetic model and Freundlich isotherm model. This work supplies a strategy for synthesizing HCPs as adsorbents for the treatment of radioactive iodine in nuclear waste .
研究领域:
材料科学
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环境科学
✓ 已验证
DOI
高影响因子
Catalysis Science & Technology
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2020
·Vol. 11
·期 1
·297-311
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IF 5.721
Xiaoqiang Zhang,Peifang Yan,Bin Zhao,Z. Conrad Zhang
The electronic and structural differences of anatase TiO2 (TiO2-A) and rutile TiO2 (TiO2-R) supported Ni catalysts are studied to understand the distinctively different catalytic pathways in guaiacol hydrodeoxygenation over Ni/TiO2-A and Ni/TiO2-R catalysts. Temperature programmed reduction profiles of NiO/TiO2-A and NiO/TiO2-R reveal two types of metal–support interactions. NiO on TiO2-R requires much higher temperature to reduce than NiO on TiO2-A by hydrogen reduction. Surface TiO2-A is partially reduced together with NiO at low temperature driven by strong interaction between reduced Ni and the reducible TiO2-A surface. In situ X-ray photoelectron spectroscopy (XPS), high resolution TEM (HRTEM), and diffuse reflectance infrared Fourier transform (DRIFT) spectroscopy of adsorbed CO reveal two types of reduced Ni species on Ni/TiO2-A: Ni0 particles and atomically dispersed electron-rich Niδ− atoms. While Ni0 particles are formed only at high Ni loadings, they are fully encapsulated by an overlayer of partially reduced TiOx, making the surface of Ni particles totally inaccessible to CO and to reactants. The electron-rich Niδ− atoms are favorably formed at all Ni loadings on the TiO2-A surface and show only linearly adsorbed CO in the DRIFT spectra. Electron transfer from Ti and O on the TiO2-A surface to atomically dispersed Ni is indicated by the observation of dominant electron-rich Niδ− species in conjunction with Ti(4+δ)+ and O(2−δ)− on Ni/TiO2-A following H2 reduction. In contrast, the chemical states of metallic Ni0 and Ti4+ remain unchanged on Ni/TiO2-R after H2 reduction. The atomically dispersed Niδ− species, formed only on the Ni/TiO2-A surface, is proposed as the active site responsible for the selective hydrodeoxygenation of guaiacol to phenolics. In contrast, the metallic Ni0 particles formed on the Ni/TiO2-R surface catalyze the typical catalytic hydrogenation, preferentially saturating the aromatic ring.
研究领域:
化学
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材料科学
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催化反应
✓ 已验证
DOI
高影响因子
Journal of Environmental Chemical Engineering
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2025
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IF 7.2
Jiahang Song,Chuanhui Shi,Yijian Zhou,Shengqian Liang,Enzhou Liu,Chen Wang,Bing Wang,Bo Zhou,Chaoyang Wei,Zhuo Li
Constructing S -scheme heterojunctions serves as a potent approach to boost photocatalytic efficiency by promoting charge transfer and attaining elevated redox potentials. Herein, a novel axially substituted subphthalocyanine derivative, H 12 SubPc-Oph-tBu (SubPc-tBu), was synthesized and assembled onto cobalt-doped ZnS (Co-ZnS) via supramolecular self-assembly to form a unique S -scheme heterojunction (SubPc-tBu/Co-ZnS). In this system, the electron-rich SubPc-tBu unit, in conjunction with the incorporated cobalt (Co), is pivotal in promoting charge transfer and enhancing the photocatalytic efficiency of the heterojunction. The photocatalyst achieved a 97 % degradation efficiency of furantoin (FT) within 30 minutes, with an apparent rate constant that is 17.24 times higher than ZnS and 10.35 times greater than SubPc-tBu, demonstrating its superior photocatalytic performance. Furthermore, after five consecutive cycles, it retained a degradation efficiency of 83.36 %, highlighting its excellent stability and recyclability. Experimental and theoretical studies revealed that the enhanced photocatalytic activity arises from an interfacial charge transfer mechanism improving carrier separation and transfer. Time-dependent density functional theory (TDDFT) and LC-MS coupled with DFT elucidated electron transfer pathways and pollutant degradation mechanisms, offering insights into photocatalyst design for environmental pollution solutions.
研究领域:
材料科学
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环境科学
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光化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）