Journal of Environmental Chemical Engineering
·
2025
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IF 7.2
Fangfang Li,Xiaofang Hou,Wei Fu,Jinjin Wang,Ying-Hua Zhou
The efficient transformation of CO 2 into high-value chemicals remains a significant challenge, particularly in the design of heterocatalysts capable of simultaneous multi-site activation towards the substrate. In this work, we develop the novel Zr-MOF catalysts incorporating both cobalt(II) meso-tetra(4-carboxyphenyl)porphine (CoTCPP) complex and the imidazolium bromide-based ionic liquid (IL) containing different alkyl chain (RImBr), where R = Et, Pr, Bu, and Pe), denoted as CoTCPP-UiO-66-IL(RImBr). The catalysts were synthesized through a solvothermal method followed by a post-synthetic modification. Among the prepared catalysts, CoTCPP-UiO-66-IL(BuImBr) demonstrated exceptional performance on the solventless and cocatalyst-free conversion of epichlorohydrin into chloropropene carbonate, achieving a remarkable 99% yield under mild conditions (90 °C and 1.0 bar CO 2 ). This outstanding catalytic efficiency was attributed to the synergistic effects of the dual Lewis-acid active sites offered by Zr-MOF node and the integrated CoTCPP complex, the strong nucleophilicity resulting from the incorporated imidazolium bromide-type IL, and the improved CO 2 adsorption capacity. Additionally, the CoTCPP-UiO-66-IL(BuImBr) catalyst exhibited excellent recyclability and broad substrate versatility in epoxide cycloaddition. These findings provide valuable insights into the development of multifunctional MOF-based heterogeneous catalysts with high activity and sustainability for CO 2 conversion applications.
研究领域:
材料科学
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催化化学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2025
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IF 6.3
Guozhu Gao,Yong Zhang,Feifei Chen,Meiqin Xu,Chang Sun,Yangfan Song,Weihua Wang,Feng Lu,Hong Dong,Hui Liu,Yahui Cheng
Copper-based catalysts have been established as highly effective for facilitating the electrochemical reduction of carbon dioxide (ECO 2 RR), particularly in the synthesis of multi-carbon (C 2+ ) compounds. However, issues of product selectivity and reaction stability persist, posing significant challenges in the context of high-current-density industrial applications. In this study, we introduce a Cu-enriched Cu 3 N composite catalyst, synthesized via a straightforward magnetron sputtering technique. This catalyst is capable of activating CO 2 and efficiently adsorbing CO, thereby enhancing the electrocatalytic performance for the targeted reactions. At a potential of −1.2 V vs. RHE, the Faradaic efficiency (FE) of the C 2+ product reaches the highest value of 80.39 % with the current density of 267.78 mA cm −2 . Remarkably, the precisely engineered catalyst architecture integrated with a metallic copper (Cu) protective layer demonstrates significantly enhanced ECO 2 RR stability, maintaining C 2+ FE above 79 % for over 10 h at 200 mA cm −2 current density. These results provide a feasible approach for designing and implementing efficient and stable ECO 2 RR catalysts to generate C 2+ products for industrial applications.
研究领域:
材料科学
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电化学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2024
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IF 10.8
Yunshuo Wu,Xuanhao Wu,Jie Fan,Haiqiang Wang,Zhongbiao Wu
Iron zeolites are promising candidates for mitigating nitrous oxide (N2O), a potent greenhouse gas and contributor to stratospheric ozone destruction. However, the atomic-level mechanisms by which different iron species, including isolated sites, clusters, and particles, participate in N2O decomposition in the presence of CO still remain poorly understood, which hinders the application of the reaction in practical technology. Herein, through experiments and density functional theory (DFT) calculations, we identified that isolated iron sites were active for N2O activation to generate adsorbed O* species, which readily reacted with CO following the Eley–Rideal (E-R) mechanism. In contrast, Fe2O3 particles exhibited a different reaction pathway, directly reacting with CO to generate oxygen vacancies (Ov), which could efficiently dissociate N2O following the Mars-van Krevelen (MvK) mechanism. Moreover, the transformation of iron oxide clusters into undercoordinated FeOx species by CO was also revealed through various techniques, such as CO-temperature-programmed reduction (TPR), and ab initio molecular dynamics (AIMD) simulations. Our study provides deeper insights into the roles of different iron species in N2O-SCR by CO, and is anticipated to facilitate the understanding of multicomponent catalysis and the design of efficient iron-containing catalysts for practical applications.
研究领域:
催化化学
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环境科学
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材料科学
✓ 已验证
DOI
PubMed
高影响因子
ACS Catalysis
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2015
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IF 9.312
Kunfeng Zhao,Hailian Tang,Botao Qiao,Lin Li,Junhu Wang
Au/γ-Fe2O3 and Au/α-Fe2O3 catalysts with identical size of Au nanoparticles, chemical state of Au species, and amount of surface OH– group were prepared. The Au/γ-Fe2O3 catalyst exhibited exceptionally high activity, regardless of the heat treatments. The CO-TPR, sequential pulse reaction, and in situ Raman spectra demonstrate that the much higher activity of Au/γ-Fe2O3 originated from its higher redox property at low temperature. Systematic study shows that this higher-redox-property-based higher activity could be extended to γ-Fe2O3-supported Pt-group metals and to other reactions that follow Mars–Van Krevelen mechanism. This finding may provide a new avenue for catalyst improvement or development by choosing the suitable crystal phase of the oxide support.
研究领域:
催化化学
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材料科学
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表面科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Catalysis
·
2020
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IF 12.35
Yang Chen,Yingxin Feng,Lin Li,Jingyue Liu,Xiaoli Pan,Wei Liu,Fenfei Wei,Yitao Cui,Botao Qiao,Xiucheng Sun,Xiaoyu Li,Jian Lin,Sen Lin,Xiaodong Wang,Tao Zhang
Exclusive Pt species supported on inert substrates have not achieved satisfactory performance for cryogenic CO oxidation because of the constraint of the competitive Langmuir–Hinshelwood process in which the strongly adsorbed CO inhibits the activation of O2. Here, we develop a catalyst of Pt nanoparticles on Al2O3 that exhibits extremely high activity with 100% CO conversion at −20 °C and orders of magnitude higher specific rate than current commercial catalysts. Detailed catalyst characterizations reveal the presence of metallic Pt sites and positively charged ones associated with the OH species in Pt/Al2O3. Both experimental data and theoretical calculations suggest that CO adsorbed on Pt(OH) kink sites reacts with OH species covering Pt0 terrace sites to release CO2. Afterward, O2 is facilely activated on terrace sites to regenerate OH. The presence of OH species and the synergy between Pt kink and terrace sites on the Pt species lead to an ultralow reaction barrier for CO oxidation.
研究领域:
催化化学
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材料科学
✓ 已验证
DOI
高影响因子
Nanoscale
·
2021
·Vol. 13
·期 14
·6856-6862
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IF 7.79
Fan Yang,Chunzheng Wu,Hongbo Yu,Shiwei Wang,Tong Li,Bo Yan,Hongfeng Yin
Nanosized Au catalysts suffer from serious sintering problems during synthesis or catalytic reactions at high temperatures. In this work, we integrate dumbbell-shaped Au–Fe3O4 heterostructures into hollow ZrO2 nanocages to make Au–Fe2O3@ZrO2 yolk–shell nanoreactors with high activity as well as ultra-high sintering resistance for high-temperature CO oxidation. The synthesis starts with the fabrication of a (Au–Fe3O4)@SiO2@ZrO2 core–shell nanostructure with a Au–Fe3O4 dumbbell nanoparticle (DB) core and SiO2/ZrO2 double shells, followed by calcination and the selective removal of the inner SiO2 shell with alkaline solution to obtain Au–Fe2O3@ZrO2 nanoreactors. The retained ZrO2 hollow (outer) shells protect the Au NPs from aggregation at temperatures up to 900 °C and show excellent long-term stability. Compared to Au@ZrO2 yolk–shell nanoreactors, Au–Fe2O3@ZrO2 shows improved activity in CO oxidation due to the active Au–Fe2O3 interface. This strategy can be extended to other yolk–shell nanoreactors with various nanocomposites and for different catalytic reactions.
研究领域:
材料科学
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催化化学
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纳米技术
✓ 已验证
DOI
高影响因子
CHEMISTRY LETTERS
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2022
·Vol. 51
·期 4
·395-398
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IF 1.715
Zhu Yue,Li Yue,Zhao Shipeng,Jing Ran,Zhang Heqian,Sun Daolai,Sato Satoshi
Hydrogenation of γ-valerolactone (GVL) to form 1,4-pentanediol (1,4-PDO) was performed over Co/ZrO2 catalysts with a Co metal loading of 15 wt. %. The calcination of Co/ZrO2 at high temperatures significantly promoted the catalytic activity irrespective of the decrease in the specific surface area. The 750 °C-calcined Co/ZrO2 with Co2+ species exhibited a high catalytic performance: a GVL conversion of 86.1% with a 1,4-PDO selectivity of 97.2% was achieved at 165 °C under 5 MPa H2 pressure.
研究领域:
化学工程
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催化科学
✓ 已验证
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2024
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IF 5.8
Jihai Zhao,Qi Wang,Yaowen Wang,Xinbo Li,Chang Liu,Taotao Huang,Liping Li,Guangshe Li
The spin state of transition metal ions, specifically controlled by the electrons in antibonding orbital, is recognized as a descriptor for heterogeneous catalysts. However, the influence of spin state on the adsorption of CO molecular with two electrons in the highest occupied molecular orbital, has been overlooked. In this work, the Co 2+ spin states in multicomponent rock-salt oxides are regulated by increasing configurational entropy, demonstrating the impact of Co 2+ spin states on CO adsorption. The CO catalytic oxidation activity of as-synthesized rock-salt oxides exhibits a volcano-shaped relationship with the ratio of Co 2+ in high spin state to Co 2+ in low spin state. Mg 0.33 Co 0.33 Ni 0.33 O with this spin state ratio of 7.5 has the largest negative adsorption energy to CO molecular and exhibits the best catalytic activity. The findings on the relationship between the spin state of transition metal ions and reactant adsorption can contribute to the understanding of catalytic activity at the electronic level.
研究领域:
材料科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
CATALYSIS LETTERS
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2024
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IF 2.3
Sun Xiaoqin,Zhang Zehua,Yun Sining
Plasmonic-driven photocatalyst have outstanding solar driven surface plasmon resonance (SPR) characteristics, and it is a prospective approach to improve photocatalytic performance. Herein, plasmonic Co metal decorated SrTiO 3 : La/Cr hollow cubes was developed and constructed by template-free hydrothermal method. The photocatalyst possesses the merits of the hollow structure with large specific surface area and strong light absorption. The intimate contact between Co and SrTiO 3 : La/Cr promotes the interfacial charge transfer. Co-SrTiO 3 : La/Cr manifests the superior photocatalytic performance toward water splitting for hydrogen evolution compared with that of other cocatalyst. And the H 2 evolution exceeds 210 μmol·g −1 ·h −1 under the optimum of the amount of 1.25wt% Co NPs. The mechanism of the enhanced performance comes from the improvement of light absorption in the visible-light region induced by SPR, as well as the efficient interfacial separation and transport of charge carriers on the photocatalyst facilitated by the local electromagnetic fields of plasmonic Co metal. Graphical Abstract
研究领域:
材料科学
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能源科学
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纳米技术
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2012
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IF 2.289
Peng Gao,Shaoqiang Yang,Zhu Xue,Guangbo Liu,Guoli Zhang,Longqiang Wang,Guobao Li,Yuzeng Sun,Yujin Chen
As a new type hydrogen storage material, Co–B hydrogen storage alloy was a hot research topic and has been paid increasing attention in recent years. In this work, a series of Co–B alloys with molar ratio of 1:1, 2:1 and 3:1 were synthesized by high energy ball-milling method. The phase, structure and morphology of the samples have been characterized by X-ray diffraction (XRD) and scanning electron microscope (SEM), which demonstrated that the samples ball-milled more than 5 h were mainly amorphous phase. Their electrochemical performance as electrochemical hydrogen storage material was investigated by galvanostatic charge–discharge process and cyclic voltammetry (CV) techniques. Electrochemical measurements showed that the Co–B alloys had excellent electrochemical hydrogen storage capacities and exhibited remarkable high rate discharge performance. Their electrochemical hydrogen storage capacity was 771 mAh/g, which was much higher than previous reports (238 mAh/g). Based on XRD and CV results, the exceptional electrochemical performances were suggested to arise from the electrochemical hydrogen storage reaction on the Co–B materials, which was brought about by the special amorphous structure and high chemical reactivity of the Co–B particles.
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
JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Ni Wang,Wenbin Li,Guiqiang Cao,Ruixian Duan,Jingjie Pei,Penghui Luo,Jianhua Zhang,Jingjing Wang,Xifei Li
ABSTRACT The “shuttle effect” caused by polysulfide (LiPSs) dissolution and diffusion is a great challenge for sulfur (S) cathode in lithium-sulfur batteries (LSBs). Herein, we have successfully constructed Co/CoV 2 O 6 tandem catalytic heterostructure anchored by N-doped carbon (Co/CoV 2 O 6 /NC) via an impregnation-assisted pyriaolysis method. The “adsorption-transfer-conversion” tandem catalytic mechanism for LiPSs is realized by utilizing the three behaviors of the strong chemical adsorption of CoV 2 O 6 to LiPSs, the strong conversion of Co to LiPSs, and the transport effect of CoV 2 O 6 ←Co interfacial built-in electric field to polysulfide ions. This can effectively suppress the “shuttle effect” by separating the adsorption and conversion process of LiPSs at different active sites. The tandem catalytic characteristic coupled with the interfacial Co-N and V-N bonds among Co, CoV 2 O 6 and NC, the high electrical conductivities of metal Co and NC conducting network, the hierarchical porous structure of polyhedral framework, collectively endow Co/CoV 2 O 6 /NC@S cathode with strong structural stability, weak electrochemical polarization, good electrochemical reversibility and fast electrochemical kinetics. As a result, Co/CoV 2 O 6 /NC@S cathode presents the significantly enhanced electrochemical performance with a high capacity of 558.4 mAh g -1 at 0.2 C after 100 cycles and a low-capacity decay rate of 0.123% per cycle during 300 cycles at 1 C.
研究领域:
材料科学
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电化学
·
能源存储
✓ 已验证
DOI
高影响因子
ACS Catalysis
·
2021
·
IF 13.084
Dongdong Chen,Huarong Lei,Wuwan Xiong,Ying Li,Xiang Ji,Jia-Yue Yang,Baoxiang Peng,Mingli Fu,Peirong Chen,Daiqi Ye
Phosphorus (P) originating from lubricant oil additives or biofuels is an emerging chemical poison in catalytic systems for automotive exhaust after-treatment. Here, we demonstrate that P-poisoning led to severe deactivation of small-pore Pd-SSZ-13 zeolites (with CHA framework) as passive NOx adsorbers (PNA) and CO oxidation catalysts for cold-start exhaust purification applications. Deactivation mechanisms of P-poisoning were unraveled by comparatively examining the P-free and P-loaded Pd-SSZ-13 zeolites using transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), nuclear magnetic resonance (NMR), temperature-programmed reduction by hydrogen (H2-TPR), CO pulse adsorption, temperature-programmed desorption using NH3 as a probe molecule (NH3-TPD), ultraviolet/visible light (UV/vis) spectroscopy, and in situ diffuse relectance infrared Fourier transform spectroscopy (DRIFTS). The loss of isolated Pd sites─namely, [Pd(OH)]+ and Pd2+ (located in the eight- and six-membered rings of CHA framework, respectively)─was revealed to be largely responsible for the deactivation of Pd-SSZ-13 in passive NOx adsorption and catalytic CO oxidation. In situ DRIFTS studies using NO or CO as a probe molecule suggest that [Pd(OH)]+ was more susceptible to P-poisoning than Pd2+. Specifically, P-poisoning led to a migration of [Pd(OH)]+ from cationic exchange sites to the zeolite surface, forming inactive metaphosphate (i.e., [Pd(OH)]+PO3–) and bulk PdOx species at high temperatures. In contrast, P-poisoning of Pd2+ sites proceeded via a sequential transformation to [Pd(OH)]+ first, and then to [Pd(OH)]+PO3– and bulk PdOx. This study provides a comprehensive mechanistic understanding on the deactivation of Pd-SSZ-13 by P-poisoning, and may guide the design of high-performance, phosphorus-resistant Pd-zeolite catalysts for cold-start exhaust after-treatment.
研究领域:
催化材料
·
环境科学
·
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）