Catalysis Science & Technology
·
2020
·Vol. 10
·期 11
·3709-3719
·
IF 5.721
Chengwei Qiu,Jinjin Lin,Jinni Shen,Dan Liu,Zizhong Zhang,Huaxiang Lin,Xuxu Wang
Anatase/rutile TiO2 heterophase junction composites have been documented to have much higher photocatalytic activity than single phase TiO2 (nude anatase or nude rutile) for various chemical reactions, including hydrogen production from methanol–water solution and pollution degradation. Further improving the photocatalytic performance of heterophase junction photocatalysts is a subject worth studying in both theory and practice. Based on the concept of junction interface regulation and our previous findings, we embedded Ni12P5 nanoparticles at the interface between anatase (A) and rutile (R) TiO2 by a multi-step preparation method to obtain an A/Ni12P5/R composite with a sandwich-like structure. It was found that loading Ni12P5 on the outside surface of anatase TiO2 (Ni12P5/A), rutile TiO2 (Ni12P5/R), P25 TiO2 (Ni12P5/P25), and A/R composite (Ni12P5/A/R) leads to a decrease in the photocatalytic activity; however, interestingly, the A/Ni12P5/R sample showed higher photocatalytic activity than the other samples of loaded or unloaded Ni12P5, although the loaded Ni12P5 in the latter case is inaccessible to the reactant molecules. This abnormal phenomenon can be attributed to two main reasons. (i) Ni12P5 as a metal-like material has a higher work function than anatase and rutile, which leads to the formation of Schottky junctions at the interface between the two intimately contacted phases. (ii) When Ni12P5 is located on the outside surface, the Schottky junction is unfavorable for the transfer of photogenerated electrons from TiO2 to Ni12P5. However, when Ni12P5 is sandwiched between A and R, the formation of a reverse tandem Schottky junction can facilitate the directed transfer of photogenerated electrons from R phase to A phase. This work again verifies that photocatalytic activity can be regulated and controlled by introducing metal and metal-like particles within the junction of a metal/semiconductor interface or even on a semiconductor/semiconductor interface. Our findings not only provide a novel usage of Ni12P5 as a co-photocatalyst but also deepens the understanding of the Schottky effect on the photocatalytic process.
研究领域:
材料科学
·
光催化
✓ 已验证
DOI
高影响因子
Atmosphere
·
2022
·Vol. 13
·期 2
·333
·
IF 3.11
Chao Wang,Lingdong Kong,Shengyan Jin,Lianghai Xia,Jie Tan,Yuwen Wang
Soot and aged soot are often found to be mixed with atmospheric particles, which inevitably affect various atmospheric heterogeneous reactions and secondary aerosol formation. Previous studies have investigated the heterogeneous reaction of NO2with different types of soot, but there are few studies on the heterogeneous reaction of NO2with mixtures containing diesel soot (DS) or aged DS and mineral dust particles. In this study, the effects of DS and aged DS on the heterogeneous reaction of NO2on the surface of γ-Al2O3were investigated via in-situ diffuse reflectance infrared Fourier transform spectrometry (DRIFTS). The results showed that the DS or DS n-hexane extract significantly inhibited the formation of nitrate on γ-Al2O3particles and promoted the formation of nitrite. At 58% RH, with the increase of DS or DS n-hexane extract loading amount, the effect of DS or DS n-hexane extract on the formation of nitrate changed from promotion to inhibition, but DS or DS n-hexane extract always promoted the formation of nitrite. The results also showed that light was conducive to the formation of nitrate on the DS-γ-Al2O3or DS-n-hexane extract-γ-Al2O3particles. Furthermore, the influence of soot aging on the heterogeneous reaction of NO2was investigated under light and no light. In the dark, O3-aged DS-γ-Al2O3or O3-aged DS-n-hexane extract-γ-Al2O3firstly inhibited the formation of nitrate on the mixed particles and then promoted it, while the effect of aged DS on nitrite formation was complex. Under light, the O3-aged DS-γ-Al2O3firstly promoted the formation of nitrate on the mixed particles and then inhibited it, while the O3-aged DS-n-hexane extract-γ-Al2O3promoted the formation of nitrate on the mixed particles. Our results further showed that the production of nitrate on the O3-aged particles under light or no light was greater than that of the UV-nitrate-aged particles. This study is helpful to deeply understand the atmospheric chemical behavior of soot and the heterogeneous conversion of atmospheric NO2.Keywords:soot;NO2;heterogeneous reaction;aged soot;γ-Al2O3
研究领域:
大气化学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
CATALYSIS LETTERS
·
2025
·Vol. 155
·期 2
·1-17
·
IF 2.4
Gan Wei,Guo Yan,Zhu Dan,Ling Min,Jiang Can,Zhang Shengfu
With the increasing problems caused by water pollution, the use of photocatalytic oxidation to remove pollutants from wastewater is a sustainable strategy. However, it is challenging to develop well-designed photocatalysts with high photo-quantum efficiency and the comprehension of their photocatalytic reaction mechanisms. Herein, a R/A-TiO 2 /Ti 3 C 2 T x (R: rutile; A: anatase) photocatalyst with different ratios of rutile and anatase phases was prepared by a facile hydrothermal method. The results showed that the number of rutile and anatase phases could be readily regulated by adjusting the dosage of titanium isopropoxide (TTIP) and Ti 3 C 2 T x . The prepared R/A-TiO 2 /Ti 3 C 2 T x -0.2 contained a mass fraction of 42% rutile phase and 58% anatase phase, with the interface between the two phases exhibited a tightly bonded structure. Meanwhile, the heterojunction between the heterophase TiO 2 and Ti 3 C 2 T x interfaces improved the photo-quantum efficiency of R/A-TiO 2 /Ti 3 C 2 T x , and the degradation efficiency of Rhodamine B (RhB) by R/A-TiO 2 /Ti 3 C 2 T x -0.2 was 77.82% in 2 h under ultraviolet light illumination. Ultimately, the active species capture experiments verified that the primary active species in the photocatalytic reaction was h + , ·OH, and·O 2 − . This work could shed light on the new approach to the rational design of high-efficiency heterophase TiO 2 -based photocatalysts. Graphical R/A-TiO 2 /Ti 3 C 2 T x photocatalysts with heterojunctions were controllably synthesized by an EDTA-2Na-assisted hydrothermal method.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Chenlu Xue,Haipeng Jiang,Chenchen Zhu,Wei Gao
AlH 3 is a promising hydrogen storage material, but poses an explosion risk when suspended in air. Herein, a low-cost and environmentally friendly composite explosion suppressant is prepared using ultrasound coupled cooling crystallization and applied to suppress AlH 3 explosions. Ultrasound-induced cavitation inhibits crystal agglomeration, resulting in fine KH 2 PO 4 crystals growing on the SiO 2 surface by heterogeneous nucleation, which significantly improves the suppression effect. The decomposition products of KH 2 PO 4 react with the flame radicals in the system to generate stable products, interrupting the chain reaction of flame radicals effectively. Furthermore, the complex mesoporous structure of SiO 2 absorbs flame radicals and increases the collision probability between the radicals and the pore walls, thus suppressing flame propagation. Our research provides an important theoretical support for the safe application of light metal hydrogen storage materials.
研究领域:
材料科学
·
能源存储
·
安全工程
✓ 已验证
产品关联
DOI
高影响因子
INORGANIC CHEMISTRY
·
2024
·
IF 4.3
Xiaoxue Ke,Changcun Tang,Renzhi Xiong,Yanhe Xiao,Baochang Cheng,Shuijin Lei
It is an important strategy to design composite materials with a special microstructure and a tunable electronic structure through structural compatibility. In this work, a novel hexagonal/cubic ZnIn2S4 polymorphic heterophase junction with a three-dimensional multihierarchical structure is successfully constructed by in situ growth of hexagonal ZnIn2S4 nanosheets on the surface of cubic ZnIn2S4 flower-like microspheres prepared by topological chemical synthesis. On the one hand, the multihierarchical architecture provides large specific surface area, abundant active sites, and excellent light trapping capability. On the other hand, the construction of a direct S-scheme heterophase junction enables the formation of a special charge-transfer channel under the force of a built-in electric field, which not only improves the separation efficiency of carriers but also ensures the stronger reaction activity of charges. The prepared ZnIn2S4 heterophase junction composite photocatalyst exhibits greatly boosted photocatalytic efficiency in rhodamine B degradation, hexavalent chromium reduction, and water splitting for hydrogen production, which are 12.3, 6.5, and 3.1 times higher than that of pure hexagonal ZnIn2S4 and 8.1, 5.1, and 2.3 times higher than that of pure cubic ZnIn2S4, respectively, demonstrating its significant potential for applications in energy and environmental fields.
研究领域:
材料科学
·
环境科学
·
能源科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL RESEARCH
·
2022
·
IF 8.431
Caixia Fu,Miao Yan,Zhuoyue Wang,Ji Li,Xiaolei Zhang,Wei Song,Zhiliang Xu,Kalpana Bhatt,Zhongming Wang,Shunni Zhu
The huge application of synthetic dyes caused a severe impact in the environment. In the present study, a physico-chemical strategy of heterogeneous-Fenton catalyzed by the natural ferrous ore has been established for toxic chemical degradation , of which the complex and high-expense repetitive pH adjustment procedures were escaping. And this natural heterogeneous catalyst also could be recycled and sustainable for toxic substances treatment involved in synergetic adsorption and oxidation. The siderite , served as an adsorbent and catalyst for the degradation of methylene blue (MB). Siderite exhibited a better adsorption capacity with a saturated adsorption capacity of ∼11.08 mg/g. Batch adsorption experiments have verified that adsorption rate and adsorption equilibrium followed pseudo-second-order rate model and Langmuir isotherm equation, respectively. The combination with H 2 O 2 , showed significant enhancement of MB degradation without any pH adjustment. The effect of siderite dosage, H 2 O 2 dosage, MB concentration, initial pH, and reaction temperature on MB degradation was investigated, which also has indicated the excellent catalytic performance of siderite. About 99.71% of MB was degraded in 480 min with initial pH of 7.0, reaction temperature of 25 °C, siderite, and H 2 O 2 dosage of 2.5 g/L and 122.38 mM, respectively. It was found that siderite could be reused and remained high degradation efficiency on MB after 5 times reutilization, which also could demonstrate the sustainable and effective process to degrade organic pollution. The generation of reactive species including ·OH and O2·- have been confirmed based on scavenger test and electron spin resonance (ESR) analysis, which was dominated by heterogeneous reaction. The possible degradation mechanisms of MB have been predicted based on spectrum scanning and GC-MS analysis. Moreover, acute toxicity assessment with marine photobacterium Vibrio fisheri was conducted to investigate the toxicity change in the adsorption/oxidation coupled process. This sustainable heterogeneous-Fenton technology has been verified as a promising and applicable process for toxic organic chemicals removal due to effective mineralization and detoxification assisted with the natural ore mineral through the simple operation and mild condtions.
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Catalysis
·
2025
·
IF 13.1
Zhitong Zhou,Weixiang Guan,Xiaoli Pan,Aiqin Wang,Tao Zhang
One-pot amination coupling of vicinal diols toward the synthesis of pyrazines provides an efficient and economically viable route to access N-heterocycles from biomass, yet the current methodology relies on a fragile homogeneous catalyst system, which limits the sustainability of the chemistry. In this work, we developed a highly efficient heterogeneous catalyst 0.8Pt/13CeO2/Al2O3 which afforded diverse substituted pyrazines from readily available vicinal diols and ammonia with a yield up to 94% under mild reaction conditions and could be reused at least 6 times without obvious activity decay. Compared to the Pt/Al2O3 catalyst, the 0.8Pt/13CeO2/Al2O3 catalyst exhibited a 30-fold faster conversion rate of diols and an increased pyrazine selectivity from 48% to 79%. Characterizations revealed that doped CeO2 improved the dispersion of Pt, increased the electron density on the Pt sites, optimized the acid/basic property of the catalyst, and enhanced the adsorption strength and dehydrogenation ability of diols. All these features contributed to the increased activity and selectivity.
研究领域:
化学工程
·
催化化学
·
生物质利用
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Energy Materials
·
2022
·
IF 6.959
Xiaoshuang Kang,Guohui Dong,Tingting Dong
In this study, TiO2 samples are synthesized through two stages including hydrolysis and calcination. It is found that the addition of HCl in the hydrolysis stage could facilitate the formation of heterophase junction TiO2. By annealing at 300 °C in an argon atmosphere, interfacial oxygen vacancies (Vo) and surface Vo (distributed in the anatase phase) can be constructed in the heterophase junction TiO2. After photocatalytic experiments, it can be found that surface Vo and interface Vo have a synergistic effect in the production of photocatalytic reactive oxygen species (ROSs). Surface Vo can enrich O2 and transmit electrons to O2 on the surface of anatase. Therefore, the enriched O2 can be converted into •O2– and 1O2 easily. The interfacial Vo not only facilitate the electron transmission between the two phases but also change the electron transfer mode from I-scheme to Z-scheme. Thus, interfacial Vo make photogenerated electrons transfer to anatase and photogenerated holes leave in the rutile. These holes in the rutile part have high oxidation potential and can better oxidize H2O (or OH–) molecules to •OH. They can also oxidize •O2– to 1O2. This work promotes the further development of defect design and application in photocatalytic materials.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
Polymers
·
2022
·Vol. 14
·期 17
·3584
·
IF 4.967
Mingpan Zhang,Fuli Wang,Xinran Shi,Jing Wei,Weixia Yan,Yihang Dong,Huiqiang Hu,Kai Wei
In this study, an iron oxide/carbon nanofibers (Fe2O3/CNFs) composite was prepared by a combination of electrospinning and hydrothermal methods. The characterization of Fe2O3/CNFs was achieved via scanning electron microscopy (SEM), infrared spectroscopy (IR), X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). It is shown that when the hydrothermal reaction time was 180 °C and the reaction time was 1 h, the Fe2O3nanoparticle size was about 90 nm with uniform distribution. The photodegradation performance applied to decolorize methyl orange (MO) was investigated by forming a heterogeneous Fenton catalytic system with hydrogen peroxide. The reaction conditions for the degradation of MO were optimized with the decolorization rate up to more than 99% within 1 h, which can decompose the dyes in water effectively. The degradation process of MO by Fenton oxidation was analyzed by a UV-visible NIR spectrophotometer, and the reaction mechanism was speculated as well.Keywords:Fe2O3;carbon nanofibers;heterogeneous Fenton;methyl orange (MO)
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Jing Luo,Chenghao Zhang,Wei Liu,Bingqi Xie,Jisong Zhang
2,2,6,6-tetramethylpiperidine-1-oxyl (TEMPO) has vital applications in the field of multiphase reaction, especially for the aerobic oxidation of alcohols. Activated carbon (AC) has a porous structure, rigid surface property, and low cost, which was the prominent carrier for TEMPO immobilization to produce the heterogeneous catalyst. However, the brilliant strategy of TEMPO immobilization on AC for long-term aerobic oxidation of alcohols was still challenging. In this work, surface-formylation and reductive amination were conducted to achieve the covalent TEMPO grafting on AC, which opened up a novel routine for surface modification and preparing heterogeneous catalysts based on carbon materials. The catalysts were packed in a micro-packed bed reactor to perform continuous aerobic oxidation of various alcohols. The catalytic performance of benzyl alcohol to benzaldehyde (turnover number: 1160.6, turnover frequency: 99.6 h −1 ) was much superior to those in the literature by using covalently grafted heterogeneous TEMPO catalysts.
研究领域:
化学工程
·
催化材料
✓ 已验证
产品关联
DOI
高影响因子
Catalysts
·
2023
·Vol. 13
·期 4
·726
·
IF 3.9
Jun Qiao,Kai Zheng,Zhiwei Lin,Huiye Jin,Wenbo Yu,Chao Shen,Aiquan Jia,Qianfeng Zhang
The exploration of inexpensive and stable heterogeneous catalysts for C–S coupling reactions remains a challenging issue. Herein, we successfully prepared a new biomass-derived copper catalyst and applied it to the selective C(sp3)–H-directed sulfonylation of ketone hydrazones with commercial sodium sulfinates. The catalyst was characterized using different spectroscopic and microscopic techniques. Importantly, the prepared biomass-supported Cu catalyst catalyzed the C–S coupling reaction with considerably high activity. A variety of aryl and alkyl sulfinates were converted to the corresponding sulfones with good yields. In particular, the heterogeneous catalyst could be recovered easily after the synthesis and consecutively used at least five times with no appreciable decrease in the catalytic activity. Lastly, the copper catalyst is expected to have further applications in organic reactions catalyzed by Cu/CuO2.Keywords:biomass-derived;copper catalysts;heterogeneous;C–S coupling
研究领域:
有机化学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
Surfaces and Interfaces
·
2025
·
IF 6.3
Chaoran Huo,Yang Wu,Ying Li,Boran Shao,Jieyu Zhang,Yibing Ma
Although the existence of surface precipitation has been reported in the literature, its solubility products ( K sp ) and formation mechanism at the interface have not been widely studied. In the present study, the precipitation of nickel ions (Ni 2+ ) on the surface of montmorillonite (Mt) in the form of Ni(OH) 2 was determined by a series of adsorption/precipitation experiments, extended X-ray absorption fine structure, X-ray powder diffraction, and high-resolution transmission electron microscopy, which analytical techniques can verify mutually. Meanwhile, the differences in K sp between the Mt-water interface (heterogeneous) and pure water (homogeneous phase) precipitation were quantitatively analyzed. A newly developed adsorption-precipitation model was constructed, and the concept of apparent solubility product ( K sp ') applicable to the heterogeneous systems was proposed. The Ni(OH) 2 K sp ' at the Mt-water interface (pH=7.0) decreased by 10–100 fold compared with K sp in pure water, and K sp ' increased with the continuous accumulation of Ni 2+ layer by layer on the surface of Mt until it returned to the value of the pure water system of K sp . These findings can not only explain the bias of pure water chemistry theory used in a multi-media environment but also predict whether Ni(OH) 2 precipitates at the Mt-water interface.
研究领域:
环境科学
·
地球化学
✓ 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）