APPLIED CATALYSIS A-GENERAL
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2025
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IF 4.8
Xinyu Liu,Chengxiong Wang,Feng Feng,Yinglong Wu,Shiying Chang,Guangxin Liu,Dong Tian,Weinan Yang,Xianming Cheng,Dongxia Yang,Kongzhai Li,Yunkun Zhao
Catalyst deactivation caused by SO 2 poisoning generally hinders commercial viability of CO oxidation catalysts in the field of industrial flue gas purification. XPS results, CO-DRIFTS spectra and DFT calculations suggested that Pt was highly-dispersed and remained the oxidative states on SnO 2 support, resulting in that the rate-determining step of CO oxidation is to clean up the adsorbed CO and PtS 2 species is readily formed in a SO 2 -contained hydrothermal environment. It predominantly maintained metallic Pt 0 in the Pt/WO 3 catalyst, thereby led to cleaning up the activated oxygen atoms as the rate-determining step. It is very difficult to remove the sulfur species in SO 2 -poisoned catalysts within 600 °C and the mechanisms of CO oxidation are not affected by SO 2 poisoning for Pt/SnO 2 and Pt/WO 3 catalysts. These findings provide some significant insights to understand the mechanisms of CO oxidation and SO 2 -tolerance.
研究领域:
催化化学
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环境科学
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理论计算化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2024
·
IF 8.4
Wenji Zheng,Xiangjun Jian,Zhengwen Shi,Ziheng Li,Xuehua Ruan,Xiaobin Jiang,Hanli Wang,Zhendong Yang,Xiangcun Li,Yan Dai,Gaohong He
Facilitated transport membrane with fixed and mobile carriers is essential yet challenging to improve the CO 2 capture. Herein, a facilitated transport membrane with continuous pathway was constructed by the in-situ interlinkage of mobile aniline with the fixed carriers distributing along electrospun polyacrylonitrile (PAN) nanofibers. In this membrane, fixed amine carriers are introduced through the alkalinous hydrolysis of PAN fibers (HPAN), and are distributed along the HPAN fibers to construct a long-range continuous transport pathway for CO 2 . The mobile aniline carriers are introduced into the interfibrous voids of the HPAN nanofibers mat (NFM) by in-situ polymerization of Poly (ethylene glycol) diacrylate (PEGDA), which interlink the fixed amine carriers to achieve the facilitated transport pathway continuous completely. And the fixed amine and mobile aniline carriers are demonstrated to co-exist in the An/PEO@HPAN membrane (NFCM) by the FTIR and XPS results. Meanwhile, the XRD and DSC results indicate that the introduction of aniline increases the free volume of PEO matrix, which is beneficial for enhancing CO 2 permeation. Therefore, the 10 wt% An/PEO@HPAN-3h NFCM presents 90.81 % and 13.15 % increases in CO 2 permeability and CO 2 /N 2 selectivity under mixed gas at 0.3 MPa in contrast with the membrane without mobile aniline carriers. Under mixed gas conditions, this NFCM exhibits CO 2 permeability of 202.93 Barrer and CO 2 /N 2 selectivity of 83.89 at 0.1 MPa, reaching the 2019 McKeown upper bound.
研究领域:
材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Catalysis
·
2022
·
IF 13.7
Xiao-Chen Sun,Kun Yuan,Wang-De Hua,Zi-Rui Gao,Qian Zhang,Chen-Yue Yuan,Hai-Chao Liu,Ya-Wen Zhang
The metal–support interface plays a crucial role in heterogeneous catalysis. The modulation of the metal–support interaction (MSI) affords the possibility of promoting the catalytic efficiency per active site. Here, we report a strategy to modulate the interfacial interaction and then optimize the interfacial activity of Co/CeO2 catalysts for the water–gas shift reaction (WGSR) by a facile NH3 treatment process for the CeO2 support. The sample of Co/800N-CeO2 treated at 800 °C exhibited the highest reaction rate of 260 μmolCO/(gCo s), which was 23.8 times higher than the rate of the untreated Co/CeO2 sample. A combination of ex situ and in situ characterizations suggested that addition of the NH3 treatment process did not only weaken the metal–support interaction between the Co species and CeO2 support to strengthen CO adsorption and CO activation ability but also induced oxygen vacancy generation under reaction conditions to accelerate H2O activation. Both worked together in promoting the catalytic efficiency for the WGSR via the carboxyl pathway at a low temperature. It was worth mentioning that the N species of the CeO2 support introduced by the NH3 treatment was removed after changing the catalyst structure under reaction conditions. The interfacial structure was robust in a 60 h test at 400 °C due to the coexistence mechanism of carboxyl and formate pathways avoiding the poisoning effect of formate species on the active sites. The construction of active interfaces could be extended to Fe/CeO2 and Ni/CeO2 catalysts and could bring great promise in the design of the interfacial structure of supported catalysts in wide applications including chemical transformation reactions and industrial catalysis.
研究领域:
催化化学
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材料科学
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能源化学
✓ 已验证
DOI
高影响因子
ACS Catalysis
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2020
·
IF 12.35
Zihao Zhang,Meizan Jing,Hao Chen,Francis Okejiri,Jixing Liu,Yan Leng,Haolan Liu,Weiyu Song,Zhaoyin Hou,Xiuyang Lu,Jie Fu,Jian Liu
The catalytic transformation of renewable fatty acids into value-added fatty alcohols without the use of gaseous hydrogen is a versatile technique for the utilization of microalgae and waste cooking oil, where Cu-based catalysts are considered to be the most suitable candidate. However, the interpretation of the structure–reactivity relationship caused by different crystal types of carriers and the metal–support interface is not well understood. Herein we synthesized ZrO2-supported Cu nanoparticle catalysts via different preparation methods and reduction temperatures under similarly exposed surface facets and Cu valency but different polymorphic phases of ZrO2 (monoclinic ZrO2: m-ZrO2; tetragonal ZrO2: t-ZrO2) and the metal–support interface. Interestingly, the as-synthesized Cu/t-ZrO2 catalysts showed remarkably better catalytic performance than Cu/m-ZrO2 for the in situ hydrogenation of lauric acid in the methanol–water system. Combined experimental and density functional theory (DFT) calculation results ascribed the lower efficiency of m-ZrO2 as a carrier to weakly adsorbed reactant and intermediate molecules as well as the absence of an oxygen vacancy in the crystal phase. The interface-rich Cu/t-ZrO2 catalysts displayed higher activity normalized to the surface-exposed Cu sites toward lauryl alcohol production than the interface-deficient counterparts. DFT calculation results further revealed that this metal–support interface plays an important role in promoting the C–O bond or H–H bond cleavage in two possible reaction routes, thus reducing the activation barrier of the overall reaction.
研究领域:
催化化学
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可再生能源
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Water Process Engineering
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2022
·
IF 7.34
K.M. Wang,Y. Shen,S.F. Jiang,Z.X. Qiu,J.H. Zhou,H.Y. Wang
This study investigated the impact of two different static biocarriers (polyvinyl chloride (PVC) and polyurethane (PU)) addition in MBR for process performance, membrane fouling and microbial community treating municipal wastewater under high and low carbon/nitrogen (C/N) ratios. The results indicated that PU biocarrier addition could help to accumulate the bacteria for nitrification and denitrification ( Tauera , Amaricoccus and Nitro spira in the mixed liquor and Solitalea and Sphingobacteriales_unclassified on the biocarrier), which slightly enhanced the total nitrogen removal especially under a low influent C/N ratio of 6.7. Additionally, the PU biocarrier addition can also alter the bulk sludge characteristics with lower soluble microbial products (SMP) concentration, lower SMP protein to carbohydrates ratio and bigger particle size, leading to lower membrane fouling propensity even under a low influent C/N ratio. PU biocarrier addition also reduced the relative abundance of extracellular polymer substances (EPS) secretion-related bacteria ( Sphingobacterials_unclassified and Ohtaekwangia ) and mitigated the membrane fouling propensity. However, this is not the case with PVC biocarrier addition, which might be due to the physical properties of the static biocarrier since PU has higher porosity, specific surface area and less negative surface zeta potential than PVC. Importantly, the static biocarrier addition can improve the nitrogen removal especially under a low influent C/N ratio and facilitate the membrane fouling control, but it depends on the physical characteristics of the biocarriers.
研究领域:
环境工程
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废水处理
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微生物学
✓ 已验证
产品关联
DOI
高影响因子
Nano Research
·
2023
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IF 9.9
Wu Yuefeng,Lu Xiaotong,Cui Pengfei,Jia Wenyu,Zhou Jun,Wang Yuan,Zahid Hussain,Wu Yuxin,Rafique Muhammad Umer,Yin Xiong,Li Baoshan,Wang Leyu,Xiang Guolei
Supported Pd catalysts show superior activities for olefin productions from alkynes through semi-hydrogenation reactions, but over-hydrogenation into alkanes highly decreases olefin selectivity. Using phenylacetylene semi-hydrogenation as a model reaction, here we explore the optimization approaches toward better Pd catalysts for alkyne semi-hydrogenation through investigating support effect and metal–support interactions. The results show that the states of Pd with supports can be tuned by varying oxide reducibility, loading ratios, and post-treatments. In our system, 0.06 wt.% Pd on rutile-TiO 2 nanorods shows the highest activity owing to the synergistic effects of single-atoms and clusters. Support reducibility can change the filling degrees of Pd 4d orbitals through varying interfacial bonding strengths, which further affect catalytic activity and selectivity.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
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2020
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IF 8.758
Qijun Pei,Teng He,Yang Yu,Zijun Jing,Jianping Guo,Lin Liu,Zhitao Xiong,Ping Chen
The strong metal–support interaction (SMSI) is of significant importance to heterogeneous catalysis. The electronic modification and encapsulation of active metals by reducible supports are the intrinsic properties of the SMSI, where the latter would decrease or even cease the catalytic activity of transition metals. Here, we demonstrate for the first time that alkalies are the functional additives that can effectively manipulate the SMSI for better hydrogenation catalysis. Specifically, both thermodynamic analyses and experimental results show that the addition of alkalies to the Ru/TiO2 catalyst could form a titanate top layer that effectively hampers the migration of TiO2–x to the surface of Ru nanoparticles. In the meantime, a substantially enhanced reduction of the support is achieved, leading to an even stronger electron donation from the support to Ru. The alkali-modified Ru/TiO2 exhibits superior low-temperature catalytic activity in the hydrogenation of aromatics, which is ca. an order of magnitude higher than that of the commercial Ru/Al2O3 catalyst and is in clear contrast to that of the neat Ru/TiO2 catalyst that shows negligible activity due to the severe encapsulation of Ru by TiO2–x.
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
PubMed
高影响因子
ACS Applied Bio Materials
·
2021
·
IF 0
Hui-Zhen Yang,Ji Zhang,Yu Guo,Lin Pu,Xiao-Qi Yu
Nonviral gene vectors with stimulus responsiveness and self-reporting properties have broad application prospects in gene therapy. Herein, we developed a nanosized reduction-responsive cationic liposomal vector formed from DNS(Zn), in which a naphthalimide–sulfonamide group was used as the glutathione (GSH)-responsive group to generate a blue fluorescence signal at 458 nm. Macrocyclic polyamine (cyclen) was used as a cationic headgroup to facilitate Zn(II) coordination, which may reduce the cytotoxicity and improve transfection efficiency. The Zn-free and nonresponsive analogues were used for comparison. Fluorescent assays revealed that the GSH response of DNS(Zn) could increase the blue fluorescence signal and improve the DNA release in cells. The title material also showed higher positive ζ-potential than its nonresponsive analogue, resulting in stronger DNA binding ability and better cellular uptake. These advantages made DNS(Zn) a good candidate for nonviral gene delivery, and the transfection efficiency in HeLa cells was distinctly higher than that of its analogue and the commercially available transfection reagent. Besides plasmid DNA, DNS(Zn) could also deliver small interfering RNA (siRNA) with good gene silencing efficiency, extending the application of the liposomes. These results suggest that DNS(Zn) can serve as a highly efficient nucleic acid delivery vector with reduction-responsive fluorescence self-reporting ability in tumor cells.
研究领域:
生物化学
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分子生物学
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基因治疗
✓ 已验证
产品关联
DOI
PubMed
Catalysis Science & Technology
·
2016
·Vol. 7
·期 1
·191-199
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IF 5.287
Zhanwei Ma,Shengli Zhao,Xiaoping Pei,Xumao Xiong,Bin Hu
Three ceria nanocrystals with different morphologies (nanocubes, nanorods, and nanoparticles) were synthesized and used as supports to evaluate the support morphology-dependent ammonia synthesis activity in the structure-sensitive ammonia synthesis reaction. The Ru/r-CeO2 catalyst shows a higher catalytic reaction rate (3830 μmol g−1 h) than that of Ru/c-CeO2 (1289 μmol g−1 h) and Ru/p-CeO2 (529 μmol g−1 h) under the reaction conditions of 400 °C, 1 MPa, and 60 mL min−1. In addition, promoters (Cs, K, and Ba) can effectively enhance the catalytic activity of the catalysts such as 2Cs–Ru/r-CeO2 (14 266 μmol g−1 h) and 2K–Ru/r-CeO2 (11 227 μmol g−1 h). The effect of the morphology of the CeO2 support on the metal–support interaction and catalytic performance of the Ru/CeO2 catalysts can be correlated to the exposed crystal planes and surface composition/electronic structure of the CeO2 support with diverse morphologies.
研究领域:
催化化学
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材料科学
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表面科学
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化学工程
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无机化学
✓ 已验证
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2024
·
IF 8.4
Yang Li,Dario R. Dekel,Xuezhong He
Amine-rich facilitated transport membranes (FTMs) attract great interest in intensifying the membrane-based CO 2 separation processes. The high-molecular-weight polyvinylamine (PVAm) polymers containing fixed-site carriers of the amino groups were used to prepare highly CO 2 -permeable membranes. The sterically hindered PVAm polymers of poly(N-methyl-N-vinylamine) and poly(N-isopropyl-N-vinylamine) were obtained by functionalization of PVAm to provide superior CO 2 solubility. By loading the mobile carriers of amino acid salt (AAS) and CO 2 -philic graphene oxide (GO), the prepared FTMs render enhanced CO 2 permeance and CO 2 /N 2 selectivity. The d-spacing of 8.8 Å and the ultramicropores of 3.5 Å from GO nanosheets provide the combination of both selective surface flow and molecular sieving mechanisms to achieve improved CO 2 permeance and CO 2 /N 2 selectivity. In addition, the intercalation of GO hinders N 2 transport through the membrane due to a longer pathway, while the mobile carriers of AAS introduced into the PVAm matrix facilitate CO 2 transport through the selective layer. Therefore, the CO 2 /N 2 selectivity of the prepared FTMs was significantly enhanced to 171 based on the intensified carrier-driving transport mechanism. It can be concluded that amine-rich membranes based on both fixed and mobile carriers of the amino groups together with intercalated GO can synergistically improve the CO 2 /N 2 separation performance, and be potentially applied for CO 2 capture from flue gas .
研究领域:
化学工程
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材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2018
·
IF 6.14
Shaodan Xu,Huanxuan Li,Jia Du,Junhong Tang,Liang Wang
We report the synthesis of subnanometric Au clusters with average diameters at 1.2 nm on a low-crystallinity CeO2 support (sub-Au/LC-CeO2), which exhibit high activities and selectivities in the aerobic oxidation of C–H bonds on a series of petroleum-derived hydrocarbons under solvent-free conditions. This phenomenon is strongly related to the maximized strong metal–support interactions between subnanometric Au and the LC-CeO2 support.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Nanoscale
·
2024
·
IF 5.8
Heyun Lin,Wenzhe Zhang,Huachen Shen,Hailing Yu,Yunlei An,Tiejun Lin,Liangshu Zhong
The catalytic behavior of CO hydrogenation can be modulated by metal–support interactions, while the role of the support remains elusive. Herein, we demonstrate that the presence of strong metal–support interactions (SMSI) depends strongly on the crystal phase of TiO2 (rutile or anatase) and the treatment conditions for the TiO2 support, which could critically control the activity and selectivity of Ru-based nanocatalysts for CO hydrogenation. High CO conversion and olefin selectivity were observed for Ru/rutile-TiO2 (Ru/r-TiO2), while catalysts supported by anatase (a-TiO2) showed almost no activity. Characterization confirmed that the SMSI effect could be neglected for Ru/r-TiO2, while it is dominant on Ru/a-TiO2 after reduction at 300 °C, resulting in the coverage of Ru nanoparticles by TiOx overlayers. Such SMSI could be suppressed by H2 treatment of the a-TiO2 support and the catalytic activity of the as-obtained Ru/a-TiO2(H2) can be greatly elevated from almost inactive to >50% CO conversion with >60% olefin selectivity. Further results indicated that the surface reducibility of the TiO2 support determines the SMSI state and catalytic performance of Ru/TiO2 in the CO hydrogenation reaction. This work offers an effective strategy to design efficient catalysts for the FTO reaction by regulating the crystal phase of the support.
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
危险品化学品经营许可证（带存储）