ACS Sustainable Chemistry & Engineering
·
2020
·
IF 7.632
Jiaxin Li,Dandan Wang,Renquan Guan,Yujun Zhang,Zhao Zhao,Hongju Zhai,Zaicheng Sun
Photocatalysis provides a sustainable route to convert N2 to NH3 with the aid of a photogenerated electron. Beyond the typical issue in the photocatalytic field, NH3 synthesis requires adsorption, activation, and hydrogenation of N2. In this report, Ni-doped TiO2 (Ni-x-TiO2) photocatalysts were fabricated by a simple sol–gel method to introduce the oxygen defects and Ni site on TiO2. The oxygen vacancy (Vo) enhances the adsorption of N2 on the catalyst surface. The Ni doping induced a defect energy level below the conduction band, which prefers to accept the photogenerated electron. The electron captured by Vo tends to transfer to the adsorbed N2 and activate N2. On the other hand, the Ni site is a typical H2 production site. It provides enough H2 for the hydrogenation of N2 to form NH3. To sum up all of these advantages, Ni-doped TiO2 displays a high NH3 production rate of 46.80 μmol·g–1·h–1 which is about 7 times higher than that of pure TiO2. This manuscript provides a potential method to design a highly efficient photocatalyst for the NH3 synthesis.
研究领域:
材料科学
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催化
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化学工程
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2021
·Vol. 11
·期 4
·2040-2046
·
IF 3.361
Yang Liu,Xin Liang,Jie Zhang,Jimmy Yun,Zuobo Yang
In this study, monodispersed NiRu nanocrystals with a diameter of 3 nm were synthesized at 90 °C via a tuning hot-inject method to lower the temperature of the organic phase synthesis of monodispersed nanomaterials. The key factor for the nanocrystalline formation of NiRu alloy nanocrystals was summarized in detail. Simultaneously, the synergistic effect of Ni and Ru in CO2 methanation was explored. Doping trace Ru can significantly improve the conversion rate of CO2 methanation and CH4 selectivity. The underlying mechanism was studied in detail via X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), temperature-programmed hydrogen reduction (H2-TPR) and desorption (H2-TPD) tests, and temperature-programmed desorption of CO2 (CO2-TPD). This study gives out a new way for the general synthesis of monodisperse nickel-based nanocrystals and provides a reference for the development and application of monodispersed nanoparticles for CO2 methanation.
研究领域:
材料科学
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催化
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纳米技术
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2021
·
IF 8.742
Chenhan Zhang,Jiahui Yan,Taotao Ji,Dongying Du,Yanwei Sun,Liangliang Liu,Xiongfu Zhang,Yi Liu
Preferred orientation represents a main concern for microstructure control and performance optimization of MOF membranes. To date, it remains a challenging task to precisely control preferred orientation of ZIF-8 membrane. Herein, we prepared highly (110)-oriented ZIF-8 membrane by oriented secondary growth. Among various elements, preparation of uniform ZIF-8 nanosheet seeds through thermal conversion of identically shaped ZIF-L precursors, spin-coating-assisted oriented deposition of (110)-oriented ZIF-8 seed layer, and controlled in-plane secondary growth at low temperature were found crucial for obtaining well-intergrown (110)-oriented ZIF-8 membrane whose H 2 /CO 2 ideal selectivity exceeded H 2 /N 2 and H 2 /CH 4 under ambient conditions, owing to preferential CO 2 adsorption capacity of not only PEI but also ZIF-8 nanosheets compared with their bulk counterparts. Our research highlighted the significance of preferred orientation regulation in tailoring the gas permeation behavior of MOF membranes.
研究领域:
材料科学
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化学工程
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膜技术
✓ 已验证
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Yongjiang Shan,Mingliang He,Fei Zhang,Yingdong Yang,Yifei Wang,Tian Gui,Yuqin Li,Zhipeng Wang,Xiangshu Chen
The deployment of green hydrogen energy plays a pivotal role in propelling sustainable development and achieving carbon neutrality. Separating H2 and CH4 is a crucial step in industrial hydrogen purification. Metal–organic framework (MOF) membranes offer vast prospects for applications in gas separation. Breaking the “trade-off” between permeance and selectivity has consistently remained a primary challenge in the realm of separation membranes. In this work, highly permeable H2 separation ZIF-8 membranes were fabricated on a vertical graphene (VG)-modified α-Al2O3 support (VG@α-Al2O3), and the VG layer can afford active sites for synthesizing ZIF-8 membranes and provide more gas transport path to reduce the mass transfer resistance. With the aid of O2 plasma in improving the hydrophilicity of the VG layer, nano-ZIF-8 crystals can be synthesized on the VG to act as seeds (ZIF-8@VG@α-Al2O3) for membrane synthesis, and green synthesis membranes were realized in aqueous solution. At 90 °C for 12 h, about 900 nm-thick membrane layers were synthesized, with a high H2 permeance of 1.8 × 10–6 mol·m–2·s–1·Pa–1 and H2/CH4 separation factor of 9.6. After the synthesis period was increased to 24 h, the denser ZIF-8 membrane resulted in a higher H2/CH4 selectivity (17.2). In contrast to the MOF membranes described in previous studies, satisfactory hydrogen permeance of ZIF-8 membranes can be achieved while maintaining high selectivity.
研究领域:
材料科学
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膜分离技术
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纳米材料
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能源化学
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环境科学
✓ 已验证
DOI
高影响因子
Catalysis Science & Technology
·
2022
·Vol. 12
·期 14
·4624-4636
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IF 6.177
Yi Yang,Weixin Qian,Haitao Zhang,Zhonghao Han,Hongfang Ma,Qiwen Sun,Weiyong Ying
FeMnxZr and FeMnxZr2Na catalysts prepared by coprecipitation and impregnation methods were applied to investigate the promoting effects of Zr on iron-based catalysts for high-temperature Fischer–Tropsch synthesis (HTFT). Ar physisorption and TEM demonstrated that Zr-promoted catalysts have a larger BET surface area and larger pore volume, which are more conducive to the distribution of active phases. Zr promoted the dispersity of iron particles and reduced the grain size of iron particles, resulting in the improvement of the FTS activity. The CO-TPD and MES results revealed that the introduction of Zr promoted the dissociative adsorption of CO, thereby promoting the formation of the active phase χ-Fe5C2 while suppressing the formation of ε′-Fe2.2C and further improving the FTS activity and the selectivity to C2=–C4= in the hydrocarbon distribution. However, the addition of an excessive amount of Zr caused the excess ZrO2 to cover the surface of the active site, inhibiting the CO dissociative adsorption and the formation of χ-Fe5C2, resulting in a decrease in the CO conversion and the selectivity to C2=–C4=. The XPS and H2-TPR results proved the interaction between Fe2O3 and ZrO2. And the Fe–ZrO2 interaction inhibited the coke deposition and aggregation of the Fe species, as confirmed by XRD and TEM, respectively. The FeMn5Zr2Na catalyst exhibited the highest C2=–C4= selectivity of 34.4% at a CO conversion of 96.3%. And FeMn5Zr2Na displayed the highest production of light olefins (441.6 g h−1 kgCat−1), which was significantly higher than FeMn2Na (162.2 g h−1 kgCat−1).
研究领域:
催化
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化学工程
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材料科学
✓ 已验证
DOI
高影响因子
CATALYSIS LETTERS
·
2022
·Vol. 153
·期 3
·921-930
·
IF 2.936
Zhang Kai,Zhang Huanling,Feng Xipan,Wang Yue,Wang Guowei,Zhu Xiaolin,Li Chunyi
The catalytic activities of metal–based catalysts are largely dependent on the properties of their supports. The support (MgO, Al 2 O 3 , MgAl 2 O 4 , SiO 2, and CeO 2 ) effect of the Sn (1.2 wt%) based catalyst for the ethylbenzene dehydrogenation reaction was firstly investigated. The supported Sn-based catalysts were characterized by NH 3 -TPD, BET, XRD, and H 2 -TPR. Among the tested catalysts, the 1.2 Sn/CeO 2 catalyst presented the most effective catalytic activity, achieving a high ethylbenzene conversion of 56.2 wt% at 600 °C. The obvious support effect should originate from the electronic interaction between Sn and supports, instead of the geometric effect resulting from different dispersion of Sn species on carriers. The high activity of the 1.2 Sn/CeO 2 catalyst was attributed to the generation of oxygen vacancies on the CeO 2 surface. A typical strong metal-support interaction (SMSI) could be found in the 1.2 Sn/CeO 2 catalyst according to the comparison of H 2 -TPR, XPS, and Raman spectra result with pure CeO 2 support. The addition of Sn further promoted the generation of more oxygen vacancies by changing the redox properties of CeO 2 , and inhibited the agglomeration of CeO 2 nanoparticles, thereby enhancing greatly the catalyst's ethylbenzene dehydrogenation activity. Graphical Abstract
研究领域:
催化
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化学工程
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Frontiers in Materials
·
2022
·
IF 3.985
Pei Mengxi,Lv Shangchun,Liu Yishui,Si Zhichun,Wu Xiaodong,Ran Rui,Weng Duan,Kang Feiyu
Photocatalytic removal of organic pollutants under solar irradiation at room temperature is considered an energy-saving technique of environmental remediation. However, photocatalysis is impeded by the poor response to visible light and fast charge recombination. In this work, sub-nano Pt/β-FeOOH quantum dots (QDs) were designed to shorten the charge migration path and obtain wide light harvesting. Interestingly, the crystalline β-FeOOH QDs can be obtained by loading sub-nano Pt particles via a reconstruction mechanism of amorphous FeOOH induced by H2 spillover, which facilitates the fast kinetics of charge transition and benefits the oxygen-rich surface of the catalyst for photocatalytic oxidation reactions. Moreover, the Pt-VO-Fe interfaces were proved to be the most active sites for the activation of O2. As a result, the catalyst exhibits a predominant photocatalytic performance in toluene oxidation, achieving a TOFPt of 0.591 min−1 at room temperature under visible light irradiation. This work provides a new perspective on the design and preparation of nanocatalysts for high-efficient photocatalysis under visible light irradiation.
研究领域:
环境科学
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催化
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材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2026
·
IF 9.2
Lei Xu,Weiyuan Li,Zewei Gao,Shuang Zhang,Chuang Dong
Bentonite is introduced for the first time to activate spontaneous hydrogen generation via aluminum hydrolysis under ambient conditions. The aluminum-based composite 90Al-6.5Bentonite-3.5Bi, wt.% was prepared through powder pressing and sintering at 650 °C under an argon atmosphere. This sample reacts with pure water within 1 s across a temperature range of 0 °C to 30 °C (approximate temperatures), achieving a 100% hydrogen conversion yield at 20 °C. The maximum hydrogen production reaches 1389.59 mL g −1 at 30 °C. The bentonite-activated hydrogen generation in air and at room temperature greatly facilitates the application of hydrogen energy in mobile scenarios.
✓ 已验证
DOI
高影响因子
CATALYSIS LETTERS
·
2021
·Vol. 151
·期 10
·3004-3010
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IF 3.186
Zhou Junjie,Huang Yu,Shen Jialu,Liu Xiang
The production of H 2 from non-fossil sources is a key research challenge to contributing solving the forthcoming energy problem. Aqueous solutions of tetrahydroxydiboron have very recently appeared as a H 2 source, from which both hydrogen atoms are provided by water, in the presence of highly sophisticated nanocatalysts. Herein, commercial and cheap Pd/C is shown to be an efficient and recyclable catalyst for H 2 evolution upon tetrahydroxydiboron hydrolysis. Graphic Abstract
研究领域:
化学
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能源科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2020
·Vol. 56
·期 7
·4666-4676
·
IF 3.553
Wang Pan,Tian Xuemin,Yan Meng,Yang Boxuan,Hua Zhongqiu
In this study, a catalytic-type combustible gas sensor was fabricated by the screen-printing method. Pt supported catalysts (Pt-HZSM5) were prepared by a wet impregnation method using HZSM5 zeolite as support. It was found that Pt-HZSM5 catalysts have a highly catalytic activity to H 2 and CO at low temperatures and a selectively and fully combustible was observed at only 150 °C. A good dispersion state of Pt nanoparticles on HZSM5 zeolite particles was beneficial for the catalytic oxidization of CO and H 2 . However, a high loading amounts lead to a poor dispersion state and a weak catalytic activity. The thick film sensor based on Pt-HZSM5 catalyst was found to be highly sensitive to combustible gas with a good linearity up to 2% and a limitation of detection (LOD) around 50 ppm. Due to the low operation temperature, a highly selectivity was obtained for CO and H 2 and no cross-sensitivity to interfering gases such as CH 4 and VOCs. It was indicated that the present developed catalytic-type gas sensors could be used for the leakage detection and monitor for H 2 and CO with a low power consumption and a good selectivity.
研究领域:
材料科学
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化学工程
·
传感器技术
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Jingsheng Xu,Zhiyuan Wang,Runguo Zheng,Hongyu Sun,Yanguo Liu,Junhua You
Ni-rich cathodes especially with Ni content over 90 % are promising next-generation cathode materials for advanced high energy lithium − ion batteries. However, in comparison with Ni ≤ 80 % Ni-rich cathodes, these ultrahigh Ni-rich materials face more severe challenges in terms of harmful H2 − H3 phase transformations and structural degradation during cycling. Herein, we present a robust surface structure composted of defect-rich disordered structures and LiF/Li 2 SiO 3 coating for stabilizing the ultrahigh Ni-rich cathode LiNi 0.96 Co 0.03 Mn 0.01 O 2 (NCM96) by modification with (NH 4 ) 2 SiF 6 . The surface disordered structures including Li/TM mixing, spinel, and rock salt structure play a crucial role in inhibiting the irreversible H2-H3 phase transition and reducing lattice volume changes by lattice coherence effect. Moreover, the disordered surface in collaboration with the co-coating restrains the rapid growth of surface rock salt phase into the bulk, enhancing structural stability. The modified sample NSF-0.5 delivers a capacity of 238 mAh/g at 0.1C and maintains a capacity retention of 88.5 % at 0.5C after 100 cycles in half cell as well as 82.3 % at 1C after 300 cycles in full cell, significantly superior to the NCM96. The findings provide a simple and cost-effective surface modification strategy to enhance the structural stability and electrochemical performance of ultrahigh nickel cathodes for high-energy density LIBs.
研究领域:
材料科学
·
电化学
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能源存储
·
锂离子电池
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固态化学
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表面工程
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电池材料
✓ 已验证
DOI
高影响因子
Catalysis Science & Technology
·
2021
·Vol. 12
·期 3
·737-749
·
IF 6.119
Zhicheng Xu,Yuran Li,Yuting Lin,Bin Wang,Panting Gao,Tingyu Zhu
The reduction of NO by CO was proposed to be applied for regeneration gas to remove NOx from industrial flue gas with activated carbon purification technology. To improve the activity and sulfur resistance for the reduction of NO by CO in regeneration gas, Cu and Fe modifications on activated carbon were investigated. And various samples were characterized by XRD, XPS, TPD, H2-TPR, in situ DRIFTS and DFT calculations to explain the reaction mechanism and poisoning mechanism. The synergistic effects of oxygen-containing functional groups and metal sites show that –COOH acts as an anchor site for metals and that C–O–C acts as a protective site for Fe3+ under a SO2 atmosphere. Cu2+ sites have a high activity at low temperatures due to the large amount of adsorbed NO and the intermediate NOx− participating in the reaction with the NOx− pathway. Fe3+ sites have a high activity at high temperatures due to the high N–O dissociation activity with the *N pathway and –NCO pathway. DFT calculations proved that the binding Cu2+ and Fe3+ sites have higher activity than free Cu2+ and Fe3+ sites. A high content of SO2 exhibits various poisoning effects, mainly including the sulfation of metal sites, deposition of S, and consumption of CO. AC-Fe-H exhibits excellent resistance and stability against SO2 and H2O due to less S deposition caused by consumption through the S–CO reaction, slight sulfation caused by the protective effect of Fe2+ and C–O–C on Fe3+ sites and better hydrophobicity.
研究领域:
环境科学
·
化学工程
·
材料科学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）