ACS Applied Engineering Materials
·
2025
·
IF 3.5
Yazhou Shuang,Fang Wang,Weihao Zhao,Hongkang Wang,Zelin Ma,Jie Jian,Shiyuan Wang,Jiulong Wang,Longyang Li,Pengfei Guo,Qian Ye,Fei Xu,Hongqiang Wang
Vanadium oxide (VOx)-based catalysts for propane (C3H8) dehydrogenation (PDH) demonstrate excellent redox properties due to the multivalent property of vanadium; however, the unsatisfactory catalytic efficiency and recondite catalytic mechanisms seriously restrict their widespread applications. Herein, we proposed the doping of cobalt oxide (CoOx) species into VOx supported on alumina for simultaneously facilitating the catalytic performance in PDH with (oxidative) and without CO2 (nonoxidative). The CoOx-doped VOx species are uniformly impregnated onto alumina supports through a ligand-free wet chemical impregnation method, without any additives. The results show that the CoOx doping modulates the electronic interactions between VOx species, thus increasing the reductive capability of the catalyst and mitigating the competitive absorption of CO2 with C3H8. Consequently, superior catalytic performances are achieved in both nonoxidative and CO2-oxidative PDH reactions compared to pristine VOx species without CoOx doping. Otherwise, the dry reforming of C3H8 is significantly inhibited compared to pristine CoOx species without VOx doping. Notably, a higher and impressive conversion rate up to 55.5% for target products (C3H6) is achieved in nonoxidative PDH compared to CO2-oxidative PDH on the CoOx-doped VOx catalyst, indicative of the competitive adsorption between reactants (CO2 and C3H8) during the catalytic process. This study provides a forward-looking mechanism to establish separate reaction pathways for each reactant (CO2 and C3H8) to improve mass transfer, thereby enhancing the efficiency of CO2-oxidative PDH.
研究领域:
催化化学
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化学工程
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材料科学
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能量转换
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多相催化
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产品关联
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2024
·
IF 11.2
Mengyao Xu,Fei Liu,Shike Liu,Jun Ma,Mengqin Yao,Xiaodan Wang,Jianxin Cao
Metal-based catalysts are prevalent in the CO 2 hydrogenation to methanol owing to their remarkable catalytic activity. Herein, Ru/In 2 O 3 catalysts with different morphologies obtained by doping Ru into In 2 O 3 with irregular, rod-like, and flower-like morphologies are used for catalytic CO 2 hydrogenation to methanol. Results indicate that the flower-like Ru/In 2 O 3 (Ru/In 2 O 3 -F) exhibits higher catalytic performance than Ru/In 2 O 3 with other morphologies, achieving a 12.9% CO 2 conversion, 74.02% methanol selectivity, and 671.36 mg MeOH ·h −1 ·g cat −1 methanol spatiotemporal yield. Furthermore, Ru/In 2 O 3 -F maintains its catalytic stability over 200 h at 5 MPa and 290 °C. The promotional effect mainly stems from the fact that electronic structure of Ru can be effectively adjusted by modulating the morphology of In 2 O 3 . The strong interaction between atomically dispersed Ru and In 2 O 3 -F enhances the structural stability of Ru, inhibiting the agglomeration of the catalyst during the reaction process. Furthermore, density-functional theory calculations reveal that highly dispersed Ru atoms not only perform efficient and rapid electronic gain and loss processes, facilitating the catalytic activation of H 2 into H intermediates. It also enables the generated reactive H to rapidly overflow to the surrounding In sites to participate in CO 2 reduction. These findings provide a theoretical basis for the development of high-performance catalysts for CO 2 hydrogenation.
研究领域:
催化
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材料科学
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化学工程
·
理论化学
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产品关联
DOI
高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2024
·
IF 3.7
Yutong Pan,Pengju Gao,Shixiong Tang,Xiaoyu Han,Ziwen Hao,Jiyi Chen,Zhenmei Zhang,Heng Zhang,Xiaohui Zi,Maoshuai Li,Shiwei Wang,Yue Wang,Xinbin Ma
This work synthesized a series of Ni/CeO 2 /Al 2 O 3 catalysts with varying CeO 2 doping amounts to enhance low-temperature CO 2 methanation. The introduction of CeO 2 weakens the interaction between Ni and Al 2 O 3 , leading to the formation of Ni-CeO 2 active sites. This results in a high dispersion of Ni and CeO 2 , improved catalyst reducibility, increased number of active sites, and enhanced the CO 2 methanation. This work further investigated the impact of WHSV and catalyst stacking configuration to enhance the reaction. When the catalyst is stacked into three segments with a temperature gradient of 330 °C, 300 °C, and 250 °C under WHSV=9000 ml·h –1 ·(g cat) –1 , the CO 2 conversion significantly increases to 95%, which is remarkably close to the thermodynamic equilibrium (96%).
研究领域:
化学工程
·
催化科学
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产品关联
DOI
高影响因子
INORGANIC CHEMISTRY
·
2022
·
IF 5.436
Zhijie Zhang,Liang Li,Ying Jiang,Jiayue Xu
Heterojunction manipulation has been deemed as a promising approach in exploring efficient photocatalysts for CO2 reduction. In this article, a novel step-scheme (S-scheme) photocatalyst of CsPbBr3 quantum dots/BiOBr nanosheets (CPB/BiOBr) was fabricated via a facile self-assembly process. The strong interaction, staggered energy band alignments, and much different Fermi levels between CsPbBr3 and BiOBr promised the formation of an S-scheme heterojunction. The resultant CPB/BiOBr heterojunction delivered remarkable photocatalytic performance in CO2 reduction, with an electron consumption rate of 72.3 μmol g–1 h–1, which was 4.1 and 5.7 times that of single CsPbBr3 and BiOBr, respectively. The superior photocatalytic performance originated from the impactful spatial separation of photoinduced electron–hole pairs, as well as the preservation of strongly reductive electrons for CO2 reduction. This work offers a rational strategy to design S-scheme heterojunctions based on lead halide perovskites, which are expected to have potential applications in the field of photocatalysis and solar energy utilization.
研究领域:
材料科学
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环境科学
·
化学工程
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DOI
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Chengqi Guo,Enhui Jiang,Qiuli Chen,Wanhe Li,Yahui Chen,Shuhan Jia,Yiying Zhou,Zhonghuan Liu,Xinyu Lin,Pengwei Huo,Chunxiang Li,Yun Hau Ng,John Charles Crittenden,Zhi Zhu,Yan Yan
Efficient photocatalytic solar CO2 reduction presents a challenge because visible-to-near-infrared (NIR) low-energy photons account for over 50% of solar energy. Consequently, they are unable to instigate the high-energy reaction necessary for dissociating C═O bonds in CO2. In this study, we present a novel methodology leveraging the often-underutilized photo-to-thermal (PTT) conversion. Our unique two-dimensional (2D) carbon layer-embedded Mo2C (Mo2C–Cx) MXene catalyst in black color showcases superior near-infrared (NIR) light absorption. This enables the efficient utilization of low-energy photons via the PTT conversion mechanism, thereby dramatically enhancing the rate of CO2 photoreduction. Under concentrated sunlight, the optimal Mo2C–C0.5 catalyst achieves CO2 reduction reaction rates of 12000–15000 μmol·g–1·h–1 to CO and 1000–3200 μmol·g–1·h–1 to CH4. Notably, the catalyst delivers solar-to-carbon fuel (STF) conversion efficiencies between 0.0108% to 0.0143% and the STFavg = 0.0123%, the highest recorded values under natural sunlight conditions. This innovative approach accentuates the exploitation of low-frequency, low-energy photons for the enhancement of photocatalytic CO2 reduction.
研究领域:
材料科学
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环境科学
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化学工程
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产品关联
DOI
PubMed
高影响因子
AICHE JOURNAL
·
2025
·
IF 4
Xinrui Liu,De Ao,Mao Ye,Zhi Wang,Zhihua Qiao,Song Zhao
Metal–organic framework (MOF) glass holds great promise for gas separation applications. However, the inherent low porosity of MOF glass poses a considerable challenge in improving membrane permeability. In this work, a self-supporting MOF crystal-glass composite (CGC) membrane was synthesized via an innovative blending and melting approach, in which ZIF-62 powder was converted into an amorphous glassy phase and ZIF-9 powder was partially flux-melted, effectively preventing the reorganization of Zn─N bonds within ZIF-62. Consequently, the composite component structure significantly enhances the porosity and permeability of the MOF glass membrane. Furthermore, the incorporation of cobalt into the membrane matrix has notably enhanced its adsorption affinity for CO 2 , thereby boosting CO 2 /CH 4 selectivity. The resultant a g [(ZIF-9) 0.2 /(ZIF-62) 0.8 ] membrane has demonstrated exceptional CO 2 permeability of 20,324 barrer and superior CO 2 /CH 4 selectivity, both surpassing the 2018 upper bound. Thus, the innovative strategy for the design of MOF CGC membranes offers effective solutions to the challenges inherent in gas separation processes.
研究领域:
材料科学
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环境科学
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化学工程
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产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2016
·
IF 7.145
Haiyang Zhang,Ruili Guo,Jinpeng Hou,Zhong Wei,Xueqin Li
In this study, a carbon nanotubes composite coated with N-isopropylacrylamide hydrogel (NIPAM-CNTs) was synthesized. Mixed-matrix membranes (MMMs) were fabricated by incorporating NIPAM-CNTs composite filler into poly(ether-block-amide) (Pebax MH 1657) matrix for efficient CO2 separation. The as-prepared NIPAM-CNTs composite filler mainly plays two roles: (i) The extraordinary smooth one-dimensional nanochannels of CNTs act as the highways to accelerate CO2 transport through membranes, increasing CO2 permeability; (ii) The NIPAM hydrogel layer coated on the outer walls of CNTs acts as the super water absorbent to increase water content of membranes, appealing both CO2 permeability and CO2/gas selectivity. MMM containing 5 wt % NIPAM-CNTs exhibited the highest CO2 permeability of 567 barrer, CO2/CH4 selectivity of 35, and CO2/N2 selectivity of 70, transcending 2008 Robeson upper bound line. The improved CO2 separation performance of MMMs is mainly attributed to the construction of the efficient CO2 transport pathways by NIPAM-CNTs. Thus, MMMs incorporated with NIPAM-CNTs composite filler can be used as an excellent membrane material for efficient CO2 separation.
研究领域:
材料科学
·
环境工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Experimental Nanoscience
·
2022
·
IF 2.024
Lijie Zhang,Ying Zhang,Hongtao Wang,Jianbing Chen,Zhongqi Cao
Electrocatalytic CO2 reduction to fuel is one of the important ways to solve energy and environmental problems. In this work, the preparation of hollow Aux-Cu2O electrocatalyst and the performance of electrocatalytic CO2 reduction to ethanol were studied. Hollow Cu2O nanospheres were prepared by a soft template method, and Aux-Cu2O composites were prepared by galvanic replacement. The characterization results of XRD and XPS reveal that Cu+ is the main chemical state of Cu in the catalysts. The results of electroactive surface area demonstrate that the electroactive surface area of Au0.51-Cu2O is the largest. The performance evaluation of electrocatalytic CO2 reduction shows that the Faraday efficiency of H2 on Au0.51-Cu2O is the lowest (∼19.5%) and the Faraday efficiency of ethanol can reach ∼18.8% at −1.2 V vs. RHE. Compared with hollow Cu2O nanospheres, Aux-Cu2O catalysts have an earlier onset for ethanol production and promote the CO2 reduction to ethanol with high efficiency, while the hydrogen evolution reaction is significantly inhibited. Our study demonstrates an effective approach to develop Cu-based electrocatalysts favourable toward ethanol in electrocatalytic CO2 reduction.
研究领域:
材料科学
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电化学
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能源与环境科学
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DOI
高影响因子
Surfaces and Interfaces
·
2025
·
IF 6.3
Jintao Zhou,Yan Liu,Chuncheng Yang,Guoyong Wang
Doping and interface engineering are both pivotal strategies for enhancing the selectivity of CO 2 reduction catalysts. However, as these strategies have often been explored independently, the question of which is more effective or whether their effects can be synergistically combined remains open. Given that doping and interfaces serve as crystallographic defects, they can be engineered to coexist within the same crystal structure. In this study, we strategically introduced both defects into a copper catalyst by modulating the indium content during crystal growth. Our investigation into the electrochemical performance of these catalysts for CO conversion reveals that while doping consistently enhances conversion selectivity, the presence of Cu/In interfaces disrupts this trend. The most promising catalyst, with 3% indium doping, demonstrated an impressive CO selectivity of 95.38±1.5% and a partial current density of -2.25 mA cm - ² at -0.8 V vs. Reversible Hydrogen Electrode (RHE). This research provides critical insights into the complex interplay between doping and interface engineering, offering a new pathway for the rational design of highly selective CO 2 reduction catalysts.
研究领域:
材料科学
·
电化学
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产品关联
DOI
高影响因子
CHEMISTRY OF MATERIALS
·
2025
·
IF 7
Beibei Sun,Cheng Zeng,Suyun Deng,Yuewen Gu,Lei Gan,Huajun Yang
The separation of C2H2/CO2 under highly humid conditions by using metal–organic frameworks (MOFs) is extremely challenging because water vapor would reduce the C2H2 adsorption capacity or even degrade the structure of MOFs. In this work, a zirconium zeolitic metal–organic framework (NNM-5) with a small aperture and large cavities exhibits commendable C2H2/CO2 selectivity (16.6 at 298 K and 1 bar) and a high uptake ratio (3.13 at 298 K and 1 bar). More importantly, NNM-5 could maintain at least five breakthrough cycles under highly humid conditions (around 100% RH) without performance degradation compared to that under dry conditions. Our studies indicate that the kinetic mechanism is the key to excellent separation performance under highly humid conditions based on the fact that the material is hydrophilic with a high water uptake, but the diffusion rate of H2O is 2 orders slower than that of C2H2 and CO2 in NNM-5.
研究领域:
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
MOLECULES
·
2024
·Vol. 29
·期 8
·1899
·
IF 4.2
Jun Wang,Shuang Fu,Peng Hou,Jun Liu,Chao Li,Hongguang Zhang,Guowei Wang
Utilizing solar energy for photocatalytic CO2reduction is an attractive research field because of its convenience, safety, and practicality. The selection of an appropriate photocatalyst is the key to achieve efficient CO2reduction. Herein, we report the synthesis of TiO2/CuPc heterojunctions by compositing CuPc with TiO2microspheres via a hydroxyl-induced self-assembly process. The experimental investigations demonstrated that the optimal TiO2/0.5CuPc photocatalyst exhibited a significantly enhanced CO2photoreduction rate up to 32.4 μmol·g−1·h−1under 300 W xenon lamp irradiation, which was 3.7 times that of the TiO2microspheres alone. The results of photoelectrochemical experiments indicated that the construction of the heterojunctions by introducing CuPc effectively promoted the separation and transport of photogenerated carriers, thus enhancing the catalytic effect of the photocatalyst.
研究领域:
材料科学
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环境科学
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产品关联
DOI
PubMed
高影响因子
ANALYST
·
2011
·Vol. 136
·期 24
·5283-5286
·
IF 3.913
Yiqun Tan,Jiancan Yu,Yuanjing Cui,Yu Yang,Zhiyu Wang,Xiaopeng Hao,Guodong Qian
A novel fluorescence chemosensor based on 2,6-dicarbonylpyridine was designed and synthesized and its photophysical properties were characterized. Upon coordination of Co2+ by the central 2,6-dicarbonylpyridinyl functional group, the chemosensor 2,6-bis(4-diphenylamino-styrylcarbonyl)pyridine (PhPy) showed nearly complete fluorescence quenching, while no fluorescence response was seen towards other competing cations. The experimental results show the chemosensor is highly selective and sensitive towards Co2+ in the presence of competing ions, even in the ppb range. Job plot analysis was carried out and the results suggested that the binding of PhPy and Co2+ was probably a 2 : 1 stoichiometry.
研究领域:
分析化学
·
材料科学
✓ 已验证
DOI
PubMed
高影响因子
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