APPLIED CATALYSIS A-GENERAL
·
2025
·
IF 4.8
Qingting Zhang,Yongbin Wu,Abouelhassan A. Gomaa,Andreas Goldbach
Supported Au catalysts are widely investigated for selective oxidation processes. Here, propylene oxidation was studied over Au nanoparticles supported on MoO 3 nanobelts. Intriguingly, the Au particles were encapsulated by MoO x layers in oxidizing atmospheres yielding Au@MoO x aggregates which signal non-classical oxidative strong metal-support interaction (SMSI) between Au and MoO 3 . The core@shell particles enhanced the acrolein selectivity of MoO 3 from 18 % up to 81 % while its formation rate accelerated more than twentyfold to 1153 µmol g cat −1 h −1 at 3 wt% Au loading and 350 °C. In situ CO DRIFTS measurements, H 2 -TPR and XPS analyses suggest that the Au@MoO x entities facilitate the transfer of MoO 3 lattice oxygen to propylene in line with the Mars-van Krevelen mechanism for acrolein formation. Apparent activation energies in the 113–163 kJ mol −1 range point to re-oxidation of the ensuing oxygen-deficient MoO x moieties as rate-limiting acrolein formation step. Consequently, the oxidative SMSI strongly promotes propylene conversion to acrolein over MoO 3 -supported Au catalysts.
研究领域:
催化化学
·
材料科学
·
表面科学
✓ 已验证
产品关联
DOI
高影响因子
Advanced Energy Materials
·
2024
·Vol. 15
·期 3
·2402295
·
IF 24.4
Songshan Zhu,Shimin Ma,Di Song,Sufang He,Yunzhu Wang,Jichang Lu,Tianhao Ai,Yongming Luo
The regulation and stabilization of strong metal-support interactions (SMSI) in high temperature hydrogen-rich reaction condition remains a huge challenge due to its structural sensitivity. Herein, tunable SMSI is constructed and stabilized on TiO 2 supported Ni catalysts by TiO 2 crystal phase engineering strategy, and then a SMSI-degree-depended ethanol stream reforming (ESR) performance is demonstrated. Rutile supported Ni exhibited a weakened SMSI with 48.6% coverage, exposing more metallic Ni and Ni-TiO 2 perimeter interface sites, and displayed exceptional H 2 yield of 4.7 mol H2 /mol ethanol and an ultra-long stability of 420 h without deactivation at 500 °C. The low reaction energy and high resistance to carbon deposition (0.9 mg c /g cat ·h) and Ni 0 sintering on Ni/r-TiO 2 catalyst explained its excellent catalytic performance. Furthermore, the effect of well-defined SMSI structures on the reaction pathway and deactivation mechanism of the ESR is clarified. This work provides a precedent for the tailor and application of SMSI in high temperature hydrogen-rich reaction conditions.
研究领域:
催化化学
·
材料科学
·
能源化学
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Zhi Hu,Zidan Zou,Aidi Xie,Chun Chen,Xiaoguang Zhu,Yunxia Zhang,Haimin Zhang,Huijun Zhao,Guozhong Wang
Ceria has been widely used as catalyst support displaying a size- or shape-dependent catalytic performance due to the strong metal-support interaction (SMSI) effect with active metal. Almost all the studies on the SMSI effect of ceria-supported metal catalysts are involved generally in gas-phase reaction, but rarely in the liquid-phase reaction system. In this work, Cu/CeO 2 -P (copper loaded on nano-polyhedral CeO 2 with (1 1 1) terminated surface) was investigated its catalytic performance on liquid-phase hydrogenation and studied the SMSI effect by comparing with the catalysts supported on nano-rod and nano-cube CeO 2 . It was found that Cu was highly dispersed on the external surface of ceria in the Cu/CeO 2 -P catalyst via a moderate SMSI effect. Furthermore, the degree of the interaction showed great influence on the chemical state of Cu species, and the ratio of (Cu + +Cu 0 )/Cu 2+ in Cu/CeO 2 -P was higher than Cu/CeO 2 -R (Cu loaded on nano-rod CeO 2 with (1 1 0) plane) and Cu/CeO 2 -C (Cu loaded on nano-cube CeO 2 with (1 0 0) facet). As a result, the Cu/CeO 2 -P catalyst showed the best catalytic performance among three types of catalysts. Based on series of catalytic investigations, the catalytic performance in liquid-phase hydrogenation was intrinsically relevant to the crystal plane effect and reduced Cu proportion induced by an appropriate SMSI effect, which was completely different from gas-phase hydrogenation.
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
PubMed
高影响因子
ACS Catalysis
·
2021
·
IF 13.084
Shaofeng Liu,Haifeng Qi,Junhui Zhou,Wei Xu,Yiming Niu,Bingsen Zhang,Yang Zhao,Wei Liu,Zhimin Ao,Zhichong Kuang,Lin Li,Meng Wang,Junhu Wang
Classical strong metal–support interaction (SMSI) has attracted intensive attention in the heterogeneous catalysis field; however, its crystalline TiOx overlayer and reversible feature often curtail the effect of classical SMSI on enhancing the catalytic performance of supported metal catalysts in oxidation reactions, especially at elevated temperatures. Here, we report the evidence that Pt nanoparticles can be encapsulated by an amorphous and permeable TiOx cover layer in Pt/TiO2 catalysts under an oxidative atmosphere, where the keys are the utilization of melamine, followed by annealing in nitrogen flow and further calcination at 800 °C in air. More importantly, the formed overlayer is stabilized against re-oxidation at 400–600 °C in air, in sharp contrast to the retreat of the TiOx overlayer by subsequent oxidation treatment in classical SMSI. Such an extraordinary strategy is further demonstrated on titania-supported Pd and Rh nanoparticles, paving a promising way for designing supported platinum group metal-based catalysts with high activity and stability.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2021
·
IF 6.609
Yishuang Wu,Zixiang Lin,Xun Zhu,Xun Hu,Mortaza Gholizadeh,Hongqi Sun,Yong Huang,Shu Zhang,Hong Zhang
Catalytic hydrogenolysis of lignin to phenolic monomers has received a lot of attention, but it is still a challenge because the cleavage of the strong C(sp 2 )-O/C bonds between structural units is usually under harsh conditions, resulting in the presence of the competing reaction of hydrogenation. Herein, hydrogenolysis of an herbaceous lignin into phenolic monomers was performed over Ru supported on various (non)-functionalized graphitized carbon nanotubes (CNT, CNT-OH, CNT-COOH, and CNT-NH 2 ), which were featured by different hydrogenation performances originally from the diverse metal-support interactions. Among the investigated supports, CNT-NH 2 enables the formation of the finest Ru nanoparticles with an average size of 1.86 nm, leading to the highest yield of phenolic monomers from lignin hydrogenolysis. The best hydrogenolysis performance of Ru@CNT-NH 2 was mainly from the partial hydrogenation of C(sp 2 )-O/C bonds to C(sp 3 )-O/C bonds in lignin, thus reducing their bond dissociation energy (BDE). The intimacy between hydrogenolysis and hydrogenation was further proved by depolymerization of a lignin β-O-4 model compound.
研究领域:
化学工程
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
Science Advances
·
2017
·Vol. 3
·期 10
·
IF 0
Hailian Tang,Yang Su,Bingsen Zhang,Adam F. Lee,Mark A. Isaacs,Karen Wilson,Lin Li,Yuegong Ren,Jiahui Huang,Masatake Haruta,Botao Qiao,Xin Liu,Changzi Jin,Dangsheng Su,Junhu Wang,Tao Zhang
Supported metal catalysts play a central role in the modern chemical industry but often exhibit poor on-stream stability. The strong metal–support interaction (SMSI) offers a route to control the structural properties of supported metals and, hence, their reactivity and stability. Conventional wisdom holds that supported Au cannot manifest a classical SMSI, which is characterized by reversible metal encapsulation by the support upon high-temperature redox treatments. We demonstrate a classical SMSI for Au/TiO2, evidenced by suppression of CO adsorption, electron transfer from TiO2 to Au nanoparticles, and gold encapsulation by a TiOx overlayer following high-temperature reduction (reversed by subsequent oxidation), akin to that observed for titania-supported platinum group metals. In the SMSI state, Au/TiO2 exhibits markedly improved stability toward CO oxidation. The SMSI extends to Au supported over other reducible oxides (Fe3O4 and CeO2) and other group IB metals (Cu and Ag) over titania. This discovery highlights the general nature of the classical SMSI and unlocks the development of thermochemically stable IB metal catalysts.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
Journal of Energy Chemistry
·
2021
·
IF 9.676
Yaoxin Wang,Jiandian Wang,Ping Zheng,Changyong Sun,Junyin Luo,Xiaowei Xie
Propane dehydrogenation (PDH) provides an alternative route for producing propylene. Herein, we demonstrates that h-BN is a promising support of Pt-based catalysts for PDH. The Pt catalysts supported on h-BN were prepared by an impregnation method using Pt(NH 3 ) 4 (NO 3 ) 2 as metal precursors. It has been found that the Pt/BN catalyst undergoing calcination and reduction is highly stable in both PDH reaction and coke-burning regeneration, together with low coke deposition and outstanding propylene selectivity (99%). Detailed characterizations reveal that the high coke resistance and high propylene selectivity of the Pt/BN catalyst are derived not only from the absence of acidity on BN support, but also from the calcination-induced and reduction-adjusted strong metal-support interaction (SMSI) between Pt and BN, which causes the partial encapsulation of Pt particles by BO x overlayers. The BO x overlayers can block the low-coordinated Pt sites and constrain Pt particles into smaller ensembles, suppressing side reactions such as cracking and deep dehydrogenation. Moreover, the BO x overlayers can effectively inhibit Pt sintering by the spatial isolation of Pt during periodic reaction-regeneration cycles. In this work, the catalyst support for PDH is expanded to nonoxide BN, and the understanding of SMSI between Pt and BN will provide rational design strategy for BN-based catalysts.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Nanoscale
·
2022
·Vol. 14
·期 9
·3579-3588
·
IF 8.307
Jianjun Zhou,Tian Wang,Cheng Cheng,Fan Pan,Yunqing Zhu,Hongrui Ma,Junfeng Niu
Electrocatalytic oxidation is regarded as an effective technique for decomposing refractory organic compounds like perfluorooctanoic acid (PFOA). However, achieving highly efficient and long-life electrodes is still a great challenge. Herein, Ti/RuO2–IrO2@Pt anodes consisting of Pt4+ and Pt0 species were fabricated by combining modified microemulsion technology with a calcination process, in which Pt nanoparticles were highly dispersed and encapsulated in Ru–Ir composite oxides to form a strong metal–support interaction (SMSI) structure. The as-constructed SMSI layer on the Ti/RuO2–IrO2@Pt anode resulted in the improvement of the charge transfer capability and also increased the degradation (99.30%) and mineralization (91.32%) of PFOA during the electrochemical oxidation process. Notably, the service lifetime of Ti/RuO2–IrO2@Pt anodes was remarkably improved from 24 to 42.3 h compared to commercial Ti/RuO2–IrO2 anodes. Moreover, the possible degradation mechanism of PFOA was also speculated through the detection of short-chain perfluorocarboxylic acids and reactive radicals. These results not only revealed that the concept and methodology of SMSI could be an effective way for constructing highly efficient and stable electrocatalysts but also greatly advanced fundamental understanding.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Catalysts
·
2020
·Vol. 10
·期 3
·355
·
IF 3.52
Wucan Liu,Yongnan Liu,Kabozya M. Mardochee,Zhikun Wang,Shucheng Wang,Wei Yu,Jianjun Zhang,Wenfeng Han
SrF2promotes the dehydrochlorination (DeHCl) of 1,1-difluoro-1-chloroethane, which is the key process for the manufacture of VDF (vinylidene fluoride), one of the most typical fluorinated monomers. However, the selectivity is low as dehydrofluorination (DeHF) to VCF (vinylidene chlorofluoride) competes with the formation of VDF. In this study, SrF2@C (SrF2embedded in carbon) and SrF2@NC (N-doped carbon) catalysts were fabricated following calcination in N2with SrC2O4, PVDF (poly vinylidene fluoride) and urea as the precursors. The catalysts were characterized by XRD, SEM, TEM, and XPS. The results show that both the calcination temperature and N-doping play an important role in the conversion of HCFC-142b and the selectivity to VDF and VCF. Calcination at elevated temperatures enhances the Sr-C interaction. For SrF2@C, improved interaction facilitates withdrawing electrons from Sr by the carbon support. By contrast, the strong interaction of Sr with N-doped carbon supply electrons from N species to Sr. The electron deficiency of Sr is favorable for the adsorption of F with higher electronegativity and consequently, DeHF reaction forming VCF. The supply of electrons to Sr by the support improves the formation of VDF (DeHCl). The present work provides a potential strategy for the improvement of selectivity to the target product.Keywords:dehydrochlorination;dehydrofluorination;metal–support interaction;strontium fluoride;vinyl difluoride
研究领域:
化学工程
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Mingjie Huang,Sisi Peng,Wei Xiang,Chen Wang,Xiaohui Wu,Juan Mao,Tao Zhou
This study has revealed how the strong metal-support interaction (SMSI) between carbon nanotubes (CNTs) and Mn 0.65 Fe 2.35 O 4 (MnFeO) in boosting peroxymonosulfate (PMS) activation for rapid sulfamethoxazole (SMX) degradation. As synergized by CNTs, the PMS-activation efficiency of MnFeO could be enhanced by>24 times, but with the similar PMS-activation mechanism. It was explored that the SMSI-induced abundant surface hydroxyl groups, in cooperation with the highly hydrophobic CNTs, favored the rapid in situ interfacial degradation of SMX. This feature also endowed the MnFeO-CNTs catalyst resistance to high salinity waters containing inorganic anions (e.g., Cl - and NO 3 – ) of weak complexing abilities. Moreover, the SMSI allowed the greatly accelerated redox cycle rate of Mn species by electron-rich CNTs, resulting in efficient PMS activation. Furthermore, the application feasibility of the MnFeO-CNTs/PMS system was demonstrated for a SMX-spiked real reverse osmosis (RO) concentrate. It was found that higher concentration of PMS could realize the complete removal of SMX, despite the existence of electron-rich tyrosine-like substances would compete with the SMX degradation in the MnFeO-CNTs/PMS system. This study demonstrated that the SMSI could boost the PMS activation , and could serve as an effective material strategy for in situ interfacial organics degradation in the high salinity wastewater.
研究领域:
环境科学
·
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Entong Ye,Fangmei Lin,Chengbin Fu,Xin Zhou,Qian Lin,Hongyan Pan,Zheng Chen
A great deal of research has been carried out on the design of Pd-based catalysts in the direct synthesis of H2O2, mainly for the purpose of improving the H2O2 selectivity by weakening the activation energy on the Pd active site and thus inhibiting the dissociation of the O–O bonds in O2*, OOH*, and HOOH*. However, this often results in insufficient activation energy for the reaction between H2 and O2 on Pd, leading to difficulties in improving both the selectivity and productivity of H2O2 simultaneously. Based on this, this study reports an efficient catalyst composed of amine-functionalized SBA-15-supported Pd. The strong metal–support interaction not only makes the PdNPs highly dispersed with more Pd active sites but also improves the stability of the catalyst. The amine group modification increases the proportion of Pd0, further enhancing Pd activity and promoting the adsorption and conversion of H2 and O2 on Pd, thereby significantly increasing H2O2 productivity. Additionally, the density-functional theory simulation results showed that due to the hydrogen-bonding force between the amine group and H2O2, this particular anchoring effect would make the hydrogenation and decomposition of H2O2 effectively suppressed. Ultimately, both the selectivity and productivity of H2O2 are improved simultaneously.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Zhefei Zhao,Xuyao Yao,Ruopeng Yu,Xingyu Luo,Minhao Chen,Xiangxiang Zhang,Yinghua Xu,Youqun Chu,Xinbiao Mao,Huajun Zheng
Electrocatalytic hydrodechlorination (EHDC) stands out as an economical and prospective technology for eliminating chlorinated organic pollutants. Single-atom catalyst engineering and metal-support interaction (MSI) offer the promising strategies for developing electrocatalysts with high atom utilization and reactivity. Herein, atomically dispersed palladium (Pd) anchored on the iron (Fe)-introduced nickel phosphide (NiFeP) support is reported. The prepared NiFeP-Pd electrode exhibits outstanding electrocatalytic activity in 4-CP removal efficiency (98.8 %) with an ultra-low dosage of Pd (0.0497 mg cm −2 ) and the highest reported MA value (446.01 min −1 g −1 ), surpassing Ni 2 P-Pd by 6.34 times. Experimental results combined with theoretical calculations suggest that the superior performance of NiFeP-Pd stems from the modulated support by Fe introduction, which not only enhances the generation of adsorbed atomic hydrogen species (H*), but also reduces the energy barrier of C-H formation on Pd sites by regulating the MSI. In addition, single-Pd-atom construction on NiFeP with good conductivity and large specific surface area makes the contributions as well.
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
危险品化学品经营许可证（带存储）