Molecular Catalysis
·
2019
·
IF 2.938
Xin Li,Haixing Wang,Peiyong Sun,Shenghong Zhang,Zhilong Yao
Cu/ZrO 2 catalysts with or without boron modification were prepared, characterized, and evaluated in the hydrogenation of sec -butyl acetate (SBA) to 2-butanol. Cu/ZrO 2 catalysts were active for the hydrogenation of SBA but suffered serious deactivation due to the leaching of Cu. Introduction of boron onto Cu/ZrO 2 catalysts improved the dispersion of Cu species, the surface Cu + /Cu 0 ratios, and the catalyst stability owing to the enhanced interaction between Cu species and support. However, it decreased the intrinsic activity of Cu towards the hydrogenation of SBA and complicated the reaction network by accelerating acid-catalyzed isomerization and transesterification processes as a result of the strengthened acidity by boron. A further kinetic analysis unravelled that the reaction orders for SBA and H 2 are 0.58 and 0.83, respectively, and the apparent activation energy is 47 kJ/mol. Such understanding of the structural evolution of CuB/ZrO 2 catalysts and the consequent catalytic performances with the B contents may provide insights useful for the design of Cu catalysts with desirable stability for hydrogenation of SBA and other esters.
研究领域:
催化化学
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材料科学
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产品关联
DOI
高影响因子
CATALYSIS LETTERS
·
2024
·
IF 2.3
Liu Hang,Liu Sixu,Liang Yaozhen,Sun Yifei,Xiong Haifeng
Palladium (Pd)-based catalysts are widely used for CO 2 hydrogenation reactions due to the capability to activate H 2 , which enhances the overall CO 2 conversion. However, most of the current Pd catalysts reported show high CO 2 conversion only at higher temperature, and the exploration of efficient catalyst enabling low temperature conversion (180–300 °C) is of importance. In this study, a series of Pd-B/ZnAl 2 O 4 catalysts were synthesized via in-situ doping, resulting in the Pd crystal transformation induced from crystal to amorphous. The catalytic hydrogenation activity of the amorphous Pd-B catalyst reaches its zenith at a Pd-B mole ratio of 1:2, accompanied by the superior catalysis stability in CO 2 hydrogenation. Various characterization techniques, including XRD, CO-DRIFTS, H 2 -TPR, XPS and TEM, were used to investigate the properties of the Pd-B/ZnAl 2 O 4 catalyst. The results showed that the Pd-B/ZnAl 2 O 4 catalyst exhibited higher dispersion and better CO 2 conversion efficiency compared to unmodified Pd catalyst. Additionally, the methanol space–time yields are nearly doubled when the B decoration is employed. At 280 °C, CO 2 conversion was improved and methanol selectivity remained at ~ 65%. This study provides valuable insights into the design and optimization of Pd-B based catalysts for CO 2 hydrogenation at low temperatures. Graphical Abstract
研究领域:
催化化学
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能源化学
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材料科学
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产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Wei Gao,Zhenyu Wang,Yongzheng Zhang,Chunyin Shen,Yanli Wang,Liang Zhan
Phenolic aerogels have addressed considerate application in fabricating lightweight ablative materials owing to their excellent characteristics of large surface area, low bulk density, and low thermal conductivity . However, unsatisfactory thermal stability still limits their extensive applications. To enhance the thermal stability, we reported a facile co-precursor strategy to prepare boron-modified phenolic aerogels, through sol–gel polymerization of phenylboronic acid and phenolic resin. The thermal stability of hybrid aerogels is remarkably enhanced, achieving a char yield of up to 64.16 % at 850 ℃ due to the much higher bonding energy of B-O bonds. The phenyl-borates structure gradually transferred into B 2 O 3 , effectively fixing the oxygen content and reducing the carbon loss during the carbonization process. Moreover, the in-situ formed phenyl-borates structure contributes to forming a denser network, which affords the hybrid aerogels with diverse properties: low density (0.31–0.34 g/cm 3 ), a hierarchical micro- meso -macro porous structure with small particle size (28.42–48.58 nm), promoted compressive strength (20.65–28.46 MPa), and excellent insulation performance (0.0406–0.0564 W/(m•k)). These integrated superiorities enable the boron-modified phenolic aerogels to perform effectively in thermal insulation fields, especially for aerospace related industry.
研究领域:
材料科学
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化学工程
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DOI
高影响因子
Frontiers of Chemical Science and Engineering
·
2020
·Vol. 15
·期 5
·1088-1098
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IF 3.552
Shang Hui,Guo Chong,Ye Pengfei,Zhang Wenhui
Catalytic hydrodesulfurization (HDS) technique is widely used for clean gasoline production. However, traditional HDS catalyst (CoMo/γ-Al 2 O 3 ) exhibits high hydrogenation performance of olefins (HYDO), resulting in the loss of gasoline octane number. To achieve high HDS/HYDO ratio, the key issue is to reduce the interaction between active metals and the support, therefore, in this research, the modified CoMo/γ-Al 2 O 3 catalysts with various boron amounts were investigated under traditional or microwave heating. The effects of preparing methods as well as boron amounts on the active phase, acidic properties and HDS catalytic activities were examined. Results show that the modification, especially under microwave treatment, can significantly weaken the interaction between the active component and the support by enlarging the surface area and pore diameter, and reducing the acidity of the support. As a result, the stacking numbers of MoS 2 slabs were obviously improved by the modification and microwave treatment, contributing to higher edge/ rim ratio, and resulting in higher HDS performance and selectivity to olefin.
研究领域:
催化化学
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能源化工
✓ 已验证
DOI
高影响因子
CHEMOSPHERE
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2022
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IF 8.943
Chen Chen,Lu-Lu Zhou,Yu-Nuo Huang,Wei-Kang Wang,Juan Xu
Biochar has been developed to activate persulfate for wastewater treatment due to its carbon essence, easily-available and low-cost. Efficiently active sites and interfacial electron transfer are highly desired for peroxydisulfate (PDS) activation. In this study, boronic ester structure and defect degree of boron-doped biochar are confirmed as activate sites to improve PDS activation. The performance of pollutants degradation is proven to have structure-activity relationships with both activate sites. Moreover, boron-doped biochar exhibits higher stability and oxidation potential by forming the surface-confined complex, promoting electron transfer from pollutants to complex. The optimized boron-doped biochar has the advantages of adapting to a broad pH range (2.9–10.0), strong resistance to Cl − and organic matters, a low activation energy of 11.22 kJ mol −1 , and achieving the decomposition of practical dyeing wastewater. Our work provides a promising approach to regulating the interfacial catalytic sites of biochar by doping heteroatom for PDS activation in practical wastewater treatment.
研究领域:
环境科学
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材料科学
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
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IF 9.965
Xuzhuo Sun,Wenhui Li,Jing Chen,Xinli Yang,Baofan Wu,Zhengxi Wang,Bo Li,Haibo Zhang
As a promising dopant , electron deficient B atom not only tunes the electronic structure of electrocatalysts for improving their intrinsic catalytic activities, but also combines with hydroxy radical as strong adsorption sites for accelerating the water dissociation during the hydrogen evolution reaction (HER). In this paper, we report an electrocatalyst based on boron-modified Ru anchored on carbon nanotubes (B-Ru@CNT) that shows impressive HER activity in acidic and alkaline media. The boron-rich closo -[B 12 H 12 ] 2- borane was selected as a moderately strong reductant for the in situ reduction of a Ru salt, which yielded B-doped Ru nanoparticles . The experimental and theoretical results indicate that the incorporation of B not only weakens the Ru-H bond and downshifts the d-bond centre of Ru from the Fermi level by reducing the electron density at Ru but also accelerates the water dissociation reaction by providing B sites, which strongly adsorb OH* intermediates, and nearby Ru sites, which act as sites for the adsorption of the H* intermediate, thus boosting the HER performance and enhancing the HER kinetics. As a result of the tuning of the electronic structure via B doping, B-Ru@CNT showed excellent HER performance, yielding overpotentials of 17 and 62 mV at a current density of 10 mA cm −2 in alkaline and acidic solutions, respectively. These results indicate that our synthetic method is a promising route to B-doped metallic Ru with enhanced pH-independent HER performance.
研究领域:
材料科学
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电化学
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催化作用
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Fundamental Research
·
2022
·
IF 0
Tianxing Yang,Rui Ma,Jiale Li,Yanan Liu,Junting Feng,Yufei He,Dianqing Li
Propane dehydrogenation (PDH) is an efficient technology for the direct production of propylene. Nevertheless, current PDH catalysts mainly rely on precious Pt or toxic Cr and especially undergo severe coke deposition. Herein, we report a Ru catalyst decorated by boron species (Ru-3B/Al 2 O 3 ), which exhibits high catalytic performance for PDH. HAADF-STEM, EELS, and CO-FTIR characterization are used to identify the surface structure of the Ru active component, which shows that the high-energy unsaturated coordination sites, including corners, edges and step atoms for Ru-3B/Al 2 O 3, are appropriately modified by BO x species. The encapsulation of high-energy active sites prone to C C cracking and deep dehydrogenation leads to higher propylene selectivity (> 95%) and strong carbon resistance ( k d 0.0007 min) over Ru-3B/Al 2 O 3 . The XPS and H 2 -TPR results show that the migration of B species is driven by the reduction of B 2 O 3 to B 2 O 2 and that the coating degree of Ru particles is controlled by the chemical valance of Ru species.
研究领域:
催化化学
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材料科学
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产品关联
DOI
CHEMICAL ENGINEERING JOURNAL
·
2022
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IF 16.744
Yihui Wang,Wen Guo,Zizheng Zhu,Kai Xu,Hongyan Zhang,Wenxian Wei,Xin Xiao,Wenjie Liang,Maoshuai He,Tingting Yu,Dongen Zhang,Hong Zhao,Xingyou Xu,Tao Yang
The research of active and efficient electrocatalysts is of great importance for the practical application of some energy conversion devices. Improving the catalytic activity and utilization efficiency of noble metal is of great importance for the practical application. Here, we report a one-pot synthesis of porous rhodium octahedra through a corner-induced-selective-deposition (CISD) process. After simple interfacial boron modification, the performances towards oxygen evolution reaction (OER), hydrogen evolution reaction (HER) and oxygen reduction reaction (ORR) in alkaline media were greatly enhanced. Especially, a small overpotential of 31 mV at 10 mA/cm 2 was achieved for HER, and a high half-wave potential of 914 mV was obtained for ORR, much better than the commercial Pt/C catalysts (55 mV, 891 mV). Density functional theory (DFT) calculation reveals that the boron incorporation optimizes the adsorption properties of catalyst surface and in turn, lowers the overpotentials for the three reactions. This work may be extended to design other nanoscale functional materials with delicate nanostructures and optimized compositions.
研究领域:
材料科学
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电化学
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催化科学
✓ 已验证
产品关联
DOI
高影响因子
Small
·
2023
·Vol. 19
·期 52
·2306014
·
IF 13.3
Songliang Liu,Hugang Zhang,Tianlun Ren,Hongjie Yu,Kai Deng,Ziqiang Wang,You Xu,Liang Wang,Hongjing Wang
2D metallene possess high surface area and excellent electron transport capability, thus enabling efficient application in oxygen reduction reaction (ORR). However, the interface regulation and electronic structure optimization of metallene are still great challenges. Herein, Pd–B/Pd hetero-metallene is constructed by interface engineering and B modification strategies for efficient electrocatalytic ORR. The 2D configuration of Pd–B/Pd hetero-metallene exposes a large number of surface atoms and unsaturated defect sites, thus providing abundant catalytic active sites and exhibiting high electron mobility. More importantly, interface engineering and B modification synergistically optimizing the electronic configuration of the metallene system. This work not only provides an effective strategy for the rational regulation of the electronic configuration of metallene, but also offers a reference for the construction of efficient ORR catalysts.
研究领域:
材料科学
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电催化
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
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IF 10.652
Suli Chen,Fan Feng,Haiying Che,Yimei Yin,Zi-Feng Ma
Practical application of solid-state batteries has been severely hindered by the relatively low ionic conductivity of electrolyte and high charge-transfer resistance between electrode and solid electrolyte . The development of novel materials and creation of new nanostructures are effective strategies to address the challenges. Here, an innovative 3D composite polymer electrolyte modified with anion-trapping boron (B-CPE) is reported for the first time as a solid electrolyte for sodium-ion batteries (SIBs). The B-CPE is prepared through in situ polymerization of polymer electrolyte inside a mechanically supporting matrix. It shows excellent ionic conductivity of 2.57 × 10 −4 S cm −1 at 40 °C, high Na + transference number of 0.66, and good interfacial compatibility with Na metal anode. Moreover, solid-state SIBs were assembled by one-step in situ solidification method to form “gentle” electrode/electrolyte contact, and it’s found that the charge-transfer efficiency has been significantly improved at the electrode/electrolyte interface as well as in cathode due to the formation of ion-conducting continuous polymer phase. Hence the B-CPE based solid-state SIBs exhibit outstanding electrochemical performances as the synergistic effect of high performance electrolyte and optimized cell structure. It delivers initial discharge capacity of 113.8 mAh g −1 and maintains 80.1% of capacity during 320 cycles under 0.2 C at 40 °C, and even 80.4% of the capacity retention after 700 cycles under 3 C. Notably, the battery achieves a significant improvement in rate capability owing to the introduction of boron moieties. This work opens new possibilities to fabricate high performance other rechargeable solid-state batteries.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子