SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Jing Yang,Heng-Quan Chen,Fen Qiao,Xifeng Zhu,Tao Wang,Wei-Ping Pan
Engineering metal-based nanoarchitectures and their atomic-scale arrangement is a promising avenue for enhanced mercury adsorbent activities. Interactions between metal single atoms and substrates result in regulated transitions between distinct reaction processes that boost mercury adsorption activity. Herein, a novel sorbent of porous Co 3 O 4 with Palladium atomic dispersed was successfully prepared by one-step pyrolysis of zeolitic imidazolate framework 67 (ZIF-67) precursors. Via engineering single Pd atoms into ZIF-derived Co 3 O 4 (Pd 1 /Co 3 O 4 -ZIF), the strong metal-support interaction (SMSI) activated the reducibility of Co 3+ in porous Co 3 O 4 to efficiently adsorb and oxidize Hg 0 , enhancing its mercury removal efficiency. Specifically, Pd 1 /Co 3 O 4 -ZIF exhibited superior sorption performance for Hg 0 over a broad range of temperatures (30–350 °C) and high gaseous hourly space velocity (about 555,500 hr −1 ) with the average Hg 0 removal efficiency higher than 98%. The strategy of constructing atomic active sites on the surface of porous metal-oxide to convert adsorbed Hg 0 into HgO is a promising approach to solve the problem that Hg 0 in flue gas is challenging to remove. Density functional theory (DFT) calculation further proved that the existence of a single Pd site on the surface of Co 3 O 4 significantly reduced the energy barrier of Hg 0 to HgO at the atomic level. This work contributed to a thorough comprehension of the structural and adsorption properties of the ZIF-derived Co 3 O 4 sorbent engineering with a single atom and enabled the efficient capture of elemental mercury in flue gas by such ZIF-derived sorbent.
研究领域:
环境科学
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材料科学
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化学工程
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产品关联
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2023
·
IF 5.2
Yan Chen,Meixia Wu,Jiang Li,Qiang Zhao,Sanbing Zhang,Yong Guo,Feng Feng,Zuopeng Li
Hydrogen, as a clean and pollution-free energy with high calorific value , is one of the best alternatives to fossil fuels. Hydrogen evolution reaction (HER), as a half reaction of electrochemical water splitting, has also received extensive attention. At present, the development of low-cost and high-performance hydrogen evolution catalysts still faces enormous challenges. In this work, we synthesized a series of RuNi/TiO 2 -oxMWCNT catalysts with different Ru and Ni ratio. After optimizing the composition and proportion, RuNi/TiO 2 -oxMWCNT with Ru:Ni=4:6 has the optimal hydrogen evolution performance. High HER performance of extremely low 14.8 mV overpotential at 10 mA·cm −2 and 38.4 mV·dec −1 Tafel slope with perfect stability is achieved, which is superior to most reported ruthenium-based catalysts and even commercial Pt/C. XPS and UPS indicates that there is a metal synergistic effect of Ru and Ni and a strong SMSI between Ru and TiO 2 in the RuNi/TiO 2 -oxMWCNT catalyst, which helps to improve hydrogen evolution performance. This study provides a pathway for the rational design of multi-component nanostructured catalysts for HER.
研究领域:
电化学
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催化
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可再生能源
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材料科学
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产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
·
IF 4.2
Hua Yang,Zhang Zhang,Yongsheng He,Peng Wang,Zhuangzhuang Ren,Lizhi Wu,Yu Tang,Li Tan
Ni-based catalysts have been widely investigated in the partial oxidation of methane (POM). However, sintering and carbon deposition are severe problems for Ni-based catalysts in the POM reaction. Here, Ni/Al2O3 catalysts with Al2O3 supports prepared by different synthesis methods are used to investigate the effect of strong metal–support interaction (SMSI) and their relationships to the catalytic performance. As a result, the different strengths of SMSI between Ni species and various Al2O3 supports contribute to generating different contents of the reduced metallic Ni0 sites in the catalysts, which affects the catalytic activity in the POM reaction obviously. The surface unsaturated pentahedral coordination Al3+ centers supply SMSI in the Ni/Al2O3-H catalyst to prevent the catalyst from sintering and coking in the POM reaction, which results in better catalytic activity and catalyst stability. A new view is provided to solve the design of stable metal oxide catalysts by utilizing their SMSI effect.
研究领域:
催化
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化学工程
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材料科学
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产品关联
DOI
高影响因子
Small
·
2026
·
IF 11.8
Jiamei Ma,Xiangyun He,Jia Huang,Xinran Pang,Tingting Zhang,Yiyun Ke,Yi Pei,Junwei Xu,Xiuzhong Fang,Xianglan Xu,Xiang Wang
Methanol steam reforming (MSR) is a promising and potential technology to supply H 2 for on-board power systems utilizing proton exchange membrane (PEM) fuel cells. Developing high-performance catalysts at low temperature is still a great challenge. Herein, CuO-supported on different AMn 2 O 5 mullites (A = Pr, Sm, Eu, Y) have been designed in this work. It has been discovered that CuO/YMn 2 O 5 demonstrates a superior H 2 production rate (219.7 µmol·g cat. −1 ·s −1 ) with ultra-low CO selectivity (0.12%) at 240°C. XAFS, XRD, Raman, FTIR, and DFT calculations have testified that abundant Cu-O-M (M═Y, Mn) interface bonds are formed as reactive sites, due to a strong metal oxide support interaction (SMOSI) occurring between CuO and YMn 2 O 5 , which is confirmed by a significant H 2 spillover effect. In situ XPS and 18 O 2 tracing have proved that the surface oxygen exchange and electron transfer rates can be accelerated, thus forming abundant active surface oxygen sites. Meanwhile, the SMOSI effect remarkably improves the contents of surface Cu 0 /Cu + and alkaline sites, and active Cu metallic surface. The synergistic interaction of these factors promotes the activation of CH 3 OH and H 2 O molecules and the generation of a great amount of reactive formate intermediates, yielding a catalyst with superior MSR performance.
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产品关联
DOI
PubMed
高影响因子
Nature Communications
·
2020
·Vol. 11
·期 1
·1-8
·
IF 12.121
Du Xiaorui,Huang Yike,Pan Xiaoli,Han Bing,Su Yang,Jiang Qike,Li Mingrun,Tang Hailian,Li Gao,Qiao Botao
The strong metal-support interaction (SMSI) has long been studied in heterogonous catalysis on account of its importance in stabilizing active metals and tuning catalytic performance. As a dynamic process taking place at the metal-support interface, the SMSI is closely related to the metal surface properties which are usually affected by the size of metal nanoparticles (NPs). In this work we report the discovery of a size effect on classical SMSI in Au/TiO 2 catalyst where larger Au particles are more prone to be encapsulated than smaller ones. A thermodynamic equilibrium model was established to describe this phenomenon. According to this finding, the catalytic performance of Au/TiO 2 catalyst with uneven size distribution can be improved by selectively encapsulating the large Au NPs in a hydrogenation reaction. This work not only brings in-depth understanding of the SMSI phenomenon and its formation mechanism, but also provides an alternative approach to refine catalyst performance.
研究领域:
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
PubMed
高影响因子
ACS Catalysis
·
2020
·
IF 12.35
Zhongjie Cai,Jiajun Dai,Wen Li,Kok Bing Tan,Zhongliang Huang,Guowu Zhan,Jiale Huang,Qingbiao Li
Utilization of CO2 and its conversion to value-added chemicals are highly desirable to alleviate the environmental concerns caused by the massive anthropogenic CO2 emission. Although In2O3/Pd have been employed as efficient catalysts for hydrogenation of CO2 to methanol, the electronic effects by strong metal–support interaction (SMSI) between Pd and In2O3 are poorly understood, which is greatly affected by the morphology of In2O3. Herein, we use MIL-68(In) nanorod as a morphological template for the synthesis of hollow In2O3 nanotubes (h-In2O3) and the preparation of supported Pd catalysts for CO2 hydrogenation to methanol. Interestingly, loading Pd on h-In2O3 showed a much higher performance than In2O3 with other morphologies, which exhibited almost unchanged CO2 conversion of 10.5%, methanol selectively of 72.4%, and methanol space-time yield of 0.53 gMeOH h–1 gcat–1 over 100 h on stream at 3 MPa and 295 °C. After in-depth characterizations, we found that the different electronic properties of Pd species on In2O3 can be finely tuned by diverse synthetic conditions, which were responsible for high activity and stability. The molar fraction of Pd2+ species in the h-In2O3/Pd catalyst reached 67.6%, 3.2 times that of the In2O3@Pd catalyst (21.3%), due to the different surface chemistry of In2O3. Density function theory results indicated that the Pd donated more electrons to the curved In2O3 (222) surface than the pristine surface, and Pd2+ was critical to facilitate H2 adsorption and formation of the surface oxygen vacancy. This work demonstrates that controlling the morphology of In2O3 can modify both the Pd electronic property and SMSI between Pd and In2O3, which are the origins of the high catalytic performance.
研究领域:
化学
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材料科学
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环境科学
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催化
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2026
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IF 12.5
Jia Li,Jian Zhang,Xiaoqiang Fu,Haina Bai,Xin Cheng,Ruoyi Li
To address the water pollution issue caused by high-generation tetracycline antibiotics (HGTs), this study constructed a multi-level platinum quantum dot-multi-walled carbon nanotube/nickel foam composite electrode (PMN), achieving efficient electrocatalytic degradation of HGTs. Through the multi-scale hierarchical structural design consisting of a nickel foam (NF) macroscale layer, a multi-walled carbon nanotube (MWCNTs) mesoscale layer, and a platinum quantum dot (Pt-QDs) microscale layer, the electrode effectively inhibits the agglomeration of Pt-QDs and promotes mass transfer. The strong metal-support interaction (SMSI) accelerates electron transfer, and calculations of differential charge density and projected density of states (PDOS) confirm that MWCNTs transfer electrons to Pt-QDs, enhancing the adsorption and activation of tigecycline (TGC) by active sites. Under optimal conditions, the TGC removal efficiency reaches 92.39% within 30 min, with an energy consumption of only 0.166 kWh/m 3 . Via active species analysis, density functional theory (DFT) calculations, and liquid chromatography-mass spectrometry (LC-MS) technology, it is revealed that the degradation process is synergistically driven by cathode-generated H*/H 2 O 2 and anode-generated ·OH/reactive chlorine species (RCS), and the degradation pathways of TGC are clarified. Cyclic experiments and biotoxicity assessments confirm that the PMN electrode exhibits excellent stability, and the toxicity of intermediates is significantly reduced. The electrode also performs stably and efficiently in a continuous-flow reactor, providing a feasible solution for the removal of HGTs in actual water bodies.
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DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2018
·Vol. 42
·期 24
·19901-19907
·
IF 3.201
Xin Wang,Yi-Fan Jiang,Ya-Nan Liu,An-Wu Xu
Because of the active components, ultra small size, and the strong metal–support interaction (SMSI) between the metal and the support, noble metal/support nanocatalysts show high catalytic activity in chemical and photochemical reactions. Palladium is one of the most extensively used noble metals due to its outstanding properties. However, the high price and the trend of aggregation are two obvious defects which prevent further application of palladium in large-scale synthesis. Herein, we chose a novel oxide component Er2O3 which can effectively reduce the aggregation of palladium nanoparticles as the support. Thus, a series of highly efficient Er2O3 nanocatalysts with low palladium loading (ranging from 1.25 wt% to 2.25 wt%) were prepared as highly efficient hydrogenation nanocatalysts. Notably, the 1.75 wt% Pd–Er2O3 achieved a remarkable turnover frequency (TOF) value of 9013 h−1 for the hydrogenation of styrene at room temperature and 1 atm H2. The sample can also catalyze the hydrogenation of a variety of functional nitroarenes with excellent catalytic properties using H2 as the reductant, which was probably attributed to the synergistic effect of the strong metal–support interaction (SMSI) and strong chemisorption of H2 on Pd–Er2O3. This work could provide a new strategy and inspiration to prepare noble metal particles loaded on oxide supports with remarkable catalytic performance for various chemical transformations.
研究领域:
催化
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化学工程
·
材料科学
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产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2022
·
IF 8.047
Beilei Cui,Hua Wang,Jinyu Han,Qingfeng Ge,Xinli Zhu
The relatively cheap and abundant Ni as a catalyst for hydrodeoxygenation (HDO) of biomass lignin-derived phenolics at 350 °C and atmospheric pressure suffers from unfavorable C-C hydrogenolysis toward CH 4 with a lower direct deoxygenation (DDO) activity. Herein, we demonstrate that the activity and selectively of Ni for HDO of m-cresol can be modified through the differences of strong metal-support interaction (SMSI) on anatase and rutile TiO 2 . Characterizations showed that the presence of SMSI depended strongly on the crystal phase of TiO 2 . The SMSI dominates on Ni/a-TiO 2 after reduction at 350 °C, resulting in Ni particles partially covered by a TiO x overlayer, and this overlayer became sufficiently thick at 650 °C, causing a significant reduction of CO chemisorption. Although the catalyst became selective for DDO to toluene, the overall HDO activity was significantly reduced because of excessive SMSI. In contrast, the Ni/r-TiO 2 catalyst reduced at 350 °C exhibited little SMSI and was active for C-C hydrogenolysis like a bare Ni catalyst. Increasing reduction temperature to 650 °C, the Ni/r-TiO 2 catalyst showed moderate SMSI and became selective to toluene through DDO while completely inhibited CH 4 formation. The toluene and total aromatics yields were 84.8 and 92.2%, respectively, at full conversion. More importantly, the turnover frequency for DDO (2.43 min −1 ) on the Ni/r-TiO 2 catalyst reduced at 650 °C was ∼40 and ∼14 times higher than that of Ni on rutile and anatase, respectively, reduced at 350 °C. This study provides an example of “Goldilocks principle” in catalysis, i.e., the best performing catalyst offers a balanced SMSI!
研究领域:
催化
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化学工程
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
ChemNanoMat
·
2022
·Vol. 8
·期 10
·e202200268
·
IF 3.82
Mengmeng Liu,Jingjing Li,Pengfei Wang,Shuai Chen,Zhengping Dong,Fengwei Zhang
Graphical The encapsulation of Pt/TiO 2 -450H catalyst with SMSI into zeolite silicalite-1 (S-1) is reported. The resulting Pt/TiO 2 @S-1 catalyst dispalyed superior catalytic performance especially for halogenated nitroaromatics and without degradation in selectivity after 7 cycles. It is attributed to the high surface area, SMSI effect in confined space and the pore structure of S-1 with selective adsorption of substrates. The encapsulation of metal nanoparticles (NPs)-based active sites and homogeneous catalysts in nanoporous materials has been of highly research focus for tuning their catalytic activity, selectivity and stability. Although the catalysts with strong metal-support interaction (SMSI) hold the reversible encapsulation feature in a certain atmosphere, there is still a lack of systematic research on them in a real confined environment. Herein, we present a highly selective and stable Pt/TiO 2 @S-1 catalyst, which is prepared by in-situ growth of classical silicalite-1 on the external surface of Pt/TiO 2 -450H pre-catalyst with SMSI effect. Encouragingly, the encapsulated 20Pt/TiO 2 @S-1 catalyst demonstrates unprecedented catalytic performance for various nitroaromatics and without any degradation in selectivity after 7 cycles (>99%) for the hydrogenation of 1-chloro-4-nitrobenzene. Such situation is attributed to the high surface area, SMSI effect in confined space as well as the pore structure of silicalite-1 with selective adsorption of substrates.
研究领域:
催化
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化学工程
·
材料科学
·
环境化学
✓ 已验证
DOI
高影响因子
Russian Journal of Physical Chemistry A
·
2019
·Vol. 93
·期 9
·1754-1761
·
IF 0.581
Yin Hu,Chen Wei,Ba Mingwei,Xie Xin,Song Weiguo
Abstract Ru/TiO 2 nanocomposite was prepared via loading the active ruthenium species on anatase TiO 2 by a simple hydrothermal approach combined with a sol–gel method. The optimal catalyst with 5.0% of Ru species showed excellent catalytic performance in the solvent-free selective hydrogenation of α-pinene with the conversion of α-pinene and selectivity to cis -pinane of 100.0 and 97.1%, respectively. It has been verified that the superior performance depends on the large amounts of acidic sites induced by HF acid and the SMSI effect between the reducible TiO 2 support and Ru species on its surface. The partial loss of its activity after five hydrogenation cycles should be due to the agglomeration of the catalyst particles and the carbon deposition on the surface. The possible hydrogenation mechanism was also discussed. This work provides an effective approach to develop a highly efficient and recyclable catalyst for the solvent-free selective hydrogenation of α-pinene.
研究领域:
催化
·
化学工程
·
材料科学
·
有机化学
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产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2021
·Vol. 45
·期 32
·14406-14413
·
IF 3.591
Yubo Liu,Guoqiang Ding,Guoping Zhao,Haohao She,Yulei Zhu,Yong Yang
Combining glucose dehydration and the subsequent hydrogenation in one pot is a preferable approach for process development as such a method allows in situ generation of the reactive intermediate to undergo further reaction without extra energy-intensive separation. Herein, phosphotungstic acid and various types of titania (anatase, rutile, P25) supported Ru-based catalysts were considered as the dehydration and hydrogenation catalysts, respectively. Modulating the different reactant media (N2, H2), various products were obtained with GBL–H2O as the solvent. A considerable yield (42%) of levulinic acid (LA) and γ-valerolactone (GVL) (40%) were obtained in nitrogen and subsequent hydrogen. Ru/TiO2 (rutile) was the favorable hydrogenation catalyst among the three types of Ru/TiO2. Meanwhile, a certain amount of sorbitol (36%) was obtained in pure hydrogen. The hydrogenation of glucose is more likely to occur than the glucose dehydration. The physicochemical properties of the catalysts were characterized by XRD, BET, TPR, STEM and in situ CO/FT-IR, and the results show that well-dispersed Ru particles are located on the rutile crystallites, which facilitated the hydrogenation of LA. A strong metal support interaction (SMSI) was responsible for the various microstructure properties and the different hydrogenation reactivity. This work allows a better understanding of the reaction paths of glucose conversion.
研究领域:
催化
·
化学工程
·
材料科学
✓ 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）