FUEL
·
2024
·
IF 6.7
Liang-Liang Zhang,Kai-Xuan Yang,Cai-Long Xue,Wan-Xi Li,Bo-Qiong Li,Yi-En Du,Yong-Qiang Chen,Ya-Jie Liu
The design of an active and sulfur-resistant catalyst for dibenzothiophene (DBT) hydrodesulfurization (HDS) in crude oil purification is highly desirable but remains a grand challenge. Here, two carbon-supported cobalt phosphide catalysts Co 2 P/C and CoP/C, and a reference sample Co/C are successfully synthesized using a metal–organic-frameworks (MOFs) precursor. A P/Co ratio dependence on crystal phases is found, leading to the formation of two pure-phase cobalt phosphide catalysts CoP/C and Co 2 P/C. Catalyst evaluation in HDS of DBT shows that the CoP/C catalyst exhibits a higher activity and stability than Co 2 P/C and Co/C, giving a 93.7 % DBT conversion with 100 h stability under 3 MPa and 380 ◦C. Moreover, a 67.4 % biphenyl yield characterizes the dominance of the direct desulfurization (DDS) pathway. The obtained catalytic performance over the CoP/C catalyst is also superior to the published cobalt phosphide catalysts. Multiple characterization techniques co-evidence that the copious specific surface area, efficient electron transport from Co to P, high thermal stability of Co nanoparticles (NPs), and strong sulfur resistance account for the enhanced catalytic performance of CoP/C. The findings of this report suggest that phosphorus-modified cobalt over the carbon support can act as a promising catalyst for the HDS of DBT.
研究领域:
催化化学
·
能源材料科学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2017
·
IF 9.446
Jia Zhao,Yi Yu,Xiaolong Xu,Shuxia Di,Bolin Wang,Hao Xu,Jun Ni,LingLing Guo,Zhiyan Pan,Xiaonian Li
High-valent Au(III) complexes have attracted much attention as catalysts in many reactions. Nevertheless Au(III) catalysts suffer from instability of the oxidized metal complexes during preparation and use. Herein, we demonstrated that Au(III) catalysts can be stabilized against reduction to metallic Au 0 by modifying supported-ionic-liquid-phase-stabilized Au(III) catalyst with CuCl 2 . It was found that the that reduced Au 0 could be re-oxidized in situ to Au 3+ species by CuCl 2 during the reaction and further stabilized by the electron transfer from Cu to these active species. When evaluated in the acetylene hydrochlorination reaction, the Au-Cu-IL/AC catalyst displayed an excellent specific activity with the turnover frequency (TOF) as high as 168.5 h −1 and more than 99.8% selectivity for the product, vinyl chloride (VCM). Furthermore, the Au-Cu-IL/AC catalyst demonstrated a stable catalytic performance with a negligible loss of C 2 H 2 conversion after 500 h under typical industrial reaction conditions for acetylene hydrochlorination. Therefore, the findings of this work provide an efficient approach for designing stable high-valent metals for long-term operation, and also pave the way for the application of Au-Cu-IL/AC catalyst in industrial VCM production.
研究领域:
化学
·
催化科学
·
材料科学
✓ 已验证
DOI
高影响因子
ChemSusChem
·
2023
·Vol. 16
·期 20
·e202300872
·
IF 8.4
Na Qin,Aojie Mao,Linqiang Li,Chao Lin,Lipeng Zhai,Jing Liu,Junhua Zou,Cheng-Xing Cui,Liwei Mi
Graphical Two novel vinylene-linked covalent organic frameworks (COFs) were rationally designed and synthesized for photocatalytic H 2 evolution from water. The corresponding excellent photocatalytic H 2 evolution performance was achieved via the rational incorporation of various cyano groups into the COF skeleton. Vinylene-linked covalent organic frameworks (COFs) have attracted enormous attention for photocatalytic H 2 evolution from water because of their fully conjugated structures, high chemical stabilities, and enhanced charge-carrier mobilities. In this work, two novel vinylene-linked COFs with tuned cyano contents were successfully synthesized and then employed as photocatalysts for H 2 generation. Notably, the photocatalytic H 2 production rate of the COF with the higher cyano content reached 73 μmol h −1 under visible light irradiation, which is 2.4 times higher than that with the lower content (30 μmol h −1 ). Both the experimental and computational results demonstrated that the rational design incorporating cyano groups into COF skeletons could precisely tune the corresponding energy levels, expand the visible-light absorption, and improve the photoinduced charge separation. This work not only provides a simple method for modulating the photocatalytic activities of COFs at the molecular level, but also affords interesting insights into the relationship between their structures and photocatalytic performance.
研究领域:
材料科学
·
化学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Di Wang,Wen Liu,Haining Wang,Shanfu Lu,Yunqi Li,Liang Luo,Linfeng Yu,Yan Xiang
The rational design of high-performance electrodes for hydrogen evolution reaction (HER) is crucial for water splitting in industrial applications. Herein, dual regulation of both mass transfer and intrinsic activity for in situ grown integrated electrodes was achieved via 3D electrode design and interfacial regulation. An innovative ruthenium (Ru)-based integrated electrode was constructed through a gravity-guided chemical vapor deposition (CVD) technique, featuring a three-dimensional carbon nanotube (CNT) network structure with embedded Ru clusters. This interlaced CNT structural configuration with high porosity and superhydrophilicity improved bubble transfer efficiency by reducing bubble coverage, bubble departure time, and bubble diameter at the reaction interface. Subsequently, the introduction of appropriate covalent Ru-O bonds on the interface of the integrated electrode boosted its intrinsic HER activity. Furthermore, DFT and AIMD calculations elucidated that the formation of covalent Ru-O bonds could reduce the adsorption and desorption of H*/OH* species, strengthen the hydrogen-bond network, and optimize the orientation of water molecules in the double electric layer (EDL). Consequently, the RuOCNT integrated electrode demonstrated a remarkably low overpotential of 41 mV at 10 mA cm −2 in a 1.0 M KOH solution and the high durability indicated by a degradation rate of only 140 μV h −1 at 100 mA cm −2 after 100 h. In addition, an in-depth analysis was carried out to distinguish the contribution of covalent Ru-O sites and electrode’s 3D structure to the boosted HER activity. This study highlighted a new approach to fabricating and understanding an efficient electrode by combining electrode engineering and active site modification to enhance HER efficiency in a mutually reinforcing manner.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
JOURNAL OF ORGANIC CHEMISTRY
·
2022
·
IF 4.198
Yi-Fan Wang,Yu-Han He,Yan Su,Yang Ji,Rui Li
A palladium complex coordinated with a chiral SIPHOS ligand was evaluated as an efficient catalyst for asymmetric hydrosilylation of β-silyl styrenes with trichlorosilane and 23 1,2-bis(silyl) chiral compounds were produced. Good to excellent enantioselectivities were observed with 1-aryl-2-silyl ethanols, where the trichlorosilyl groups of the hydrosilylation products were selectively converted into a hydroxyl group in the presence of pre-installed trialkylsilyl groups. Asymmetric hydrosilylation of β-silyl styrenes followed by methylation of the trichlorosilyl group gave stable 1,2-bis(silyl) chiral compounds 4 with excellent yields. DFT calculations of hydridopalladium B coordinated with a SIPHOS ligand, an intermediate of the hydrosilylation reaction, established the optical structures to be energy minima, and the structural information could well illustrate the enantioselectivity for the hydrosilylation reaction.
研究领域:
有机化学
·
催化化学
·
理论计算化学
✓ 已验证
DOI
高影响因子
JOURNAL OF ORGANIC CHEMISTRY
·
2024
·
IF 3.3
Yue Zhang,Ting Wang,Yuan-Yuan Liu,Zheng-Bing Zhang,Pan Han,Linhai Jing
Geminal and vicinal borosilanes have unique applications in functional materials and synthetic transformations. Herein, a convenient method for the synthesis of geminal and vicinal borosilanes is developed via photoredox metal-free hydrosilylation of vinylboronic esters. This strategy features the advantages of high atom economy, environmental friendliness, and excellent functional group compatibility. The mechanism studies reveal that the catalytic reaction goes through photoredox HAT catalysis and a radical addition pathway.
研究领域:
有机化学
·
材料科学
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF SOLID STATE CHEMISTRY
·
2017
·
IF 2.299
Jian Zeng,Wangdong Zeng,Heping Zeng
Photocatalytic hydrogen generation is a considerable promising technology to decrease climate change effect of CO 2 and to solve the increasing global demand for clean energy. Hydrogen generation driven by visible light still faces many challenges although great efforts have been made. Efficient charge separation plays an important role in solar-energy conversion by heterojunction photocatalysts . Herein we report that nickel ferrites covered by gold plasmonics form well-defined plasmonic photocatalysts for fluorescein-sensitized hydrogen production under visible-light irradiation with largely enhanced photoactivity due to fast separation of photogenerated electron-hole pairs. The optimal Au/NiFe 2 O 4 plasmonic photocatalysts with AuNP loading of 1.5 wt% shows the hydrogen production rate of 0.256 mmol g −1 h −1 via localized surface plasmon resonance effect of AuNPs . Fluorescein was acted as photosensitizer to extend the visible-light absorption of Au/NiFe 2 O 4 plasmonic photocatalysts and enhance photocatalytic hydrogen generation efficiency under visible-light irradiation. The optimum rate for hydrogen generation reached 3.162 mmol g −1 h −1 and the rate is about 60-fold and 12-fold higher than that of pure NiFe 2 O 4 and 1.5 wt% Au/NiFe 2 O 4 plasmonic photocatalysts, respectively.
研究领域:
材料科学
·
能源化学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Bowen Lu,Ziqiang Han,Xinyu Zhi,Liqi Zhang
NiFe 2 O 4 exhibits excellent redox properties and is widely applied in catalytic reactions. However, rapid inactivation under reaction conditions limited its industrial applications. In this study, CeO 2 -NiFe 2 O 4 composite catalysts were synthesized, and the Reverse Water Gas Shift (RWGS) reaction was measured to reveal its CO 2 hydrogenation performance under a high-temperature condition. NiFe 2 O 4 catalysts got deactivated after being reduced to Fe-Ni alloy at 700 °C, decreasing the CO 2 conversion rate. CeO 2 addition can significantly improve its high-temperature activity, and 20CeO 2 -NiFe 2 O 4 exhibited the best catalytic activity (80.85 %, 700 °C). The CeO 2 -confined maintained Ni-Fe alloy with a relatively small crystal size and larger specific surface area, supporting more active sites for CO 2 hydrogenation. CeO 2 addition induced higher oxygen vacancy concentration, enhancing CO 2 activation and formates species formed on 20CeO 2 -NiFe 2 O 4 , resulting in higher CO 2 conversion activity. In addition, 20CeO 2 -NiFe 2 O 4 maintained its catalytic stability for 50 h at 700 °C. The CeO 2 confined enhanced the high-temperature stability of Fe-Ni alloy. CeO 2 and formed CeFeO 3 dispersed in 20CeO 2 -NiFe 2 O 4 inhibited excessive aggregation of Fe-Ni alloy, and CeO 2 inhibited carbon deposition on Fe-Ni alloy, improving Fe-Ni alloy’s reaction stability under RWGS reaction conditions. CeO 2 confined may give insight into improving metal stability under high-temperature and reductive conditions in heterogeneous catalysis.
研究领域:
催化化学
·
材料科学
·
环境科学
✓ 已验证
DOI
高影响因子
POLYMER DEGRADATION AND STABILITY
·
2024
·
IF 6.3
Sohail Yasin,Jianfeng Shi,Sheng Ye,Song Yihu,Aman Ullah,Guangzhong Li,Wenzhu Peng,Chaohua Gu
Additives play a crucial role in modifying and enhancing the properties of rubbers, improving mechanical strength, thermal stability, and chemical resistance to make them more suitable for various applications. The rubber industry faces challenges related to high resource consumption and toxic emissions, which are further impacted by the use of performance-enhancing additives. In hydrogen storage systems, tailored additives are required for rubbers to withstand elevated temperatures and high pressures, preventing hydrogen-induced swelling, a major cause of sealing failure. Herein, a novel form of carbonaceous material, carbon nano-onions (CNOs), and the bio-based plasticizer additive epoxidized soybean oil (ESO) are utilized in conventional silica-filled nitrile butadiene rubber (NBR) nanocomposites to develop low-carbon manufacturing high pressure hydrogen resistant O-rings for sealing applications. The results reveal that the incorporation of CNOs increases the crosslinking density ( v c ), assisted by ESO, in silica-filled NBR nanocomposites. While the conventional adipate-based plasticizer and ESO were found to be susceptible to high pressure hydrogen exposures, ESO demonstrated sustained compressive sealing properties with increase in von-Mises stress and in elevated thermo-oxidative conditions over time. The results of the life cycle assessment (LCA) recommend ESO for low-carbon manufacturing in rubber processing over conventional plasticizer.
研究领域:
材料科学
·
环境科学
·
能源工程
✓ 已验证
DOI
高影响因子
TALANTA
·
2024
·
IF 5.6
Shuang Meng,Xuanting He,Boyu Li,Yuanyuan Yang,Shun Mao,Zhuo Li
The excessive presence of the metal ions Cu 2+ and Fe 3+ in the environment poses a serious threat to ecosystems and human health, so timely and accurate detection of them has become essential and urgent. In this paper, a novel hydrogel-based fluorescent sensor, named ME-IPA@SA-TbZn, was fabricated facilely through an in-situ cross-linking modification method and was used for the detection of Cu 2+ and Fe 3+ in water bodies. The ME-IPA@SA-TbZn is essentially a hybrid hydrogel bead that exhibits vibrant fluorescence, employing Tb and Zn functionalized hydrogen-bonded organic frameworks (HOFs) as the fluorescence functional core and sodium alginate (SA) as the hydrogel matrix. The synthesized hydrogel sensor ME-IPA@SA-TbZn exhibits remarkable capabilities in detecting and distinguishing between Cu 2+ and Fe 3+ with high selectivity and sensitivity. Specifically, it achieves limits of detection (LODs) of 1.275 μM for Cu 2+ and 0.549 μM for Fe 3+ , respectively, both are below the maximum allowable concentrations set by the U.S. Environmental Protection Agency (EPA) for drinking water. Importantly, the hydrogel sensing platform delivers intuitive and visible results under simple operating conditions, and has been successfully applied to Cu 2+ and Fe 3+ detection in river samples. In addition, it was demonstrated that disruption of the “antenna” effect, absorption competition quenching (ACQ) effect, and ion exchange (IE) effect are the main mechanisms leading to fluorescence quenching. Based on these results, ME-IPA@SA-TbZn hold promise as a fluorescent sensor for detecting Cu 2+ and Fe 3+ ions.
研究领域:
环境科学
·
材料科学
·
分析化学
✓ 已验证
DOI
PubMed
高影响因子
ACTA PHYSICO-CHIMICA SINICA
·
2024
·
IF 10.8
Hailian Tang,Siyuan Chen,Qiaoyun Liu,Guoyi Bai,Botao Qiao,Fei Liu
The strong metal-support interaction (SMSI) is a widely recognized concept in heterogeneous catalysis, known for significantly enhancing catalyst stability and potentially modulating catalytic performance. However, because the SMSI effect is generally reversible, it tends to diminish under redox conditions opposite to those used for its construction. Consequently, its application is typically limited to conditions that are the same or similar to those under which it was formed. Herein, we report the application of oxidative SMSI (O-SMSI) constructed on hydroxyapatite-supported Rh catalyst (Rh/HAP) in a reductive reaction, the hydrogenation of furfuryl alcohol. In situ diffuse reflectance infrared Fourier transform spectroscopy of CO adsorption and electron microscopy measurements reveal that high-temperature oxidation treatment at 500 °C induced the occurrence of O-SMSI on the Rh/HAP catalyst, accompanied by the encapsulation of Rh particles by the support. Upon the O-SMSI, the Rh species were effectively stabilized on the support surface, with significant suppression of sintering and leaching during liquid-phase reactions. As a result, the catalyst showed stable furfuryl alcohol conversion and cyclopentanone selectivity during recycling tests. Furthermore, it was found that the O-SMSI and the associated encapsulation behavior on the Rh/HAP system were only partially reversible rather than completely reversible. Even after high-temperature reduction at up to 600 °C, a portion of the SMSI effect remains, ensuring the stability of the catalysts in reductive reactions. This discovery greatly expands the application scope of SMSI catalysts and provides a new way to prepare stable hydrogenation catalysts.
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2024
·
IF 4.7
Xin-Hao Shen,Feng Liu,Qin-Qin Chen,Ying Gao,Xiao-Wen Wang,Xin Liu
The efficient degradation of emerging pollutants in water, represented by CBZ, is receiving increasing attention from all sectors of society. Although advanced oxidation reactions represented by Fenton reaction can efficiently degrade emerging pollutants, the problem of iron sludge that comes with it is hindering the further promotion of this technology. Herein, UiO-66(Zr)-2OH material was synthesized by hydrothermal method and loaded with Pd 0 NPs on the surface of the material by in situ reduction. The MOFs-H 2 -Accelerated Catalytic Fenton system was constructed by accelerating the regeneration of Fe(II) in the system by activating the [H] produced by H 2 introduced into the system at room temperature and pressure. Within 180 min, the removal of the target pollutant CZB could reach more than 99 % under the condition of only 25 µmol of Fe(II) and 25 mmol of H 2 O 2 .
研究领域:
环境科学
·
材料科学
·
化学工程
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）