CHEMICAL ENGINEERING JOURNAL
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2019
·
IF 8.355
Meisheng Zhang,Baofang Jin,Yan Liu,Wei Liu,Duan Weng,Xiaodong Wu,Shuang Liu
In this work, O 3 activation was performed at 200 °C over two types of Ag/CeO 2 catalysts with nanocube- and nanorod-like morphologies, respectively. The O 3 -indcued surface O x − species (“O x − injection”) accelerated soot combustion over both catalysts temporarily. In contrast, the depletion of CeO 2 surface oxygen vacancies (Ce 3+ -V O-s ) caused by ozonization conferred to long-term activation. Specifically, the ozonized nanocubic Ag/CeO 2 with low initial Ce 3+ content not only benefited more from the “O x − injection”, but also exhibited good redox stability and high practical potential. Therefore, the combination of this catalyst with O 3 activation may result in efficient soot elimination in the particulate filters of vehicles.
研究领域:
催化
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环境科学
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材料科学
✓ 已验证
DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-12
·
IF 14.7
Ren Yuqi,Fu Yiwei,Li Naixu,You Changjun,Huang Jie,Huang Kai,Sun Zhenkun,Zhou Jiancheng,Si Yitao,Zhu Yuanhao,Chen Wenshuai,Duan Lunbo,Liu Maochang
H 2 O dissociation plays a crucial role in solar-driven catalytic CO 2 methanation, demanding high temperature even for solar-to-chemical conversion efficiencies <1% with modest product selectivity. Herein, we report an oxygen-vacancy (V o ) rich CeO 2 catalyst with single-atom Ni anchored around its surface V o sites by replacing Ce atoms to promote H 2 O dissociation and achieve effective photothermal CO 2 reduction under concentrated light irradiation. The high photon flux reduces the apparent activation energy for CH 4 production and prevents V o from depletion. The defects coordinated with single-atom Ni, significantly promote the capture of charges and local phonons at the Ni d -impurity orbitals, thereby inducing more effective H 2 O activation. The catalyst presents a CH 4 yield of 192.75 µmol/cm 2 /h, with a solar-to-chemical efficiency of 1.14% and a selectivity ~100%. The mechanistic insights uncovered in this study should help further the development of H 2 O-activating catalysts for CO 2 reduction and thereby expedite the practical utilization of solar-to-chemical technologies.
研究领域:
催化
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太阳能
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化学工程
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Yingying Jin,Kaihao Fan,Miao Feng,Yaoguang Wang,Hongfeng Chen,Xuesong Liu
This study investigates synergistic effects in Ni/CeO 2 catalysts for ammonia decomposition, comparing impregnation and mechanical mixing preparation methods. The impregnated catalyst achieved >90 % NH 3 conversion above 500 °C, outperforming Ni/SiO 2 and mixed counterparts. Strong interactions at the Ni-CeO 2 interface facilitated the formation of Ni-O-Ce bonds, lattice distortion, and oxygen vacancies (O v )/Ce 3+ species, enhancing Ni dispersion (34.7 nm vs. 73.1 nm) and electron transfer. Optimal NH 3 pretreatment (550 °C, 1.5 h) generated metallic Ni 0 as the primary active species, with higher Ni 0 content (XPS) and reducibility (H 2 -TPR). The novelty lies in establishing how NH 3 pretreatment dynamically assembles contiguous Ce 3+ -O v -Ni 0 triads. These sites facilitate rate-limiting N 2 desorption through localized electron donation from O v and Ce 3+ to Ni 0 , which weakens N-N bonds (NH 3 -TPD). Impregnation-derived synergy: (i) enhances Ni dispersion/reduction, (ii) promotes O v formation, and (iii) enables NH 3 -pretreatment-induced assembly of contiguous Ce 3+ -O v -Ni 0 triads that create electron-rich sites, lowering the activation barrier. This work provides a foundation for designing cost-effective catalysts via atomic-scale control of metal-support interactions.
研究领域:
催化
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材料科学
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化学工程
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表面科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Songlei Mo,Jia Kou,Jianrong Zeng,Kepeng Song,Yayun Zhang,Shangming He,Yongfeng Hu,Yong Guo,Xiaohui Liu,Xi Chen,Yanqin Wang
Upcycling polyethylene terephthalate (PET) wastes into high value-added oxygenated chemicals is desirable, yet it remains challenging. Herein, we develop a novel strategy to convert PET into 1,4-cyclohexanedimethanol (CHDM) via two steps, the conversion of PET to dimethyl 1,4-cyclohexanedicarboxylate (DMCD) over Ni-based catalysts, followed by the hydrogenolysis of DMCD to CHDM over a CuMgAl catalyst. The key step is the production of DMCD from PET in one-pot reaction and an unprecedent yield of 86.5% DMCD yield is achieved over Pd-modified Ni/CeO 2 catalyst, which to the best of our knowledge is the highest yield reported to date. Comprehensive characterizations demonstrate that the addition of Pd enhances hydrogen dissociation, but weakens the adsorption activation ability for C–O bond in esters, thus DMCD selectivity is improved. Over CuMgAl catalyst, DMCD is directly converted into CHDM with 83.8% yield. Furthermore, the techno-economic analysis proves the economic feasibility of converting PET into CHDM via our proposed strategy. The study provides a promising and effective approach to upcycle PET wastes into high value-added products.
研究领域:
化学工程
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催化
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废物管理
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可持续化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2019
·
IF 6.97
Kirill A. Alferov,Zhongwei Fu,Shuxian Ye,Dongmei Han,Shuanjin Wang,Min Xiao,Yuezhong Meng
A new one-pot synthesis method of dimethyl hexane-1,6-diyldicarbamate (HDC), a potential intermediate compound in the synthesis of polyurethanes, from CO2, methanol, and 1,6-hexanediamine (HDA) is disclosed. The starting materials are renewable, stable, easily available, and cheap. The process was implemented in 1-methyl-2-pyrrolidinone (NMP) solvent over CeO2 catalysts. Three different CeO2 catalysts (commercial nanospheres, CeO2(c) obtained by direct calcination of (NH4)2Ce(NO3)6, and CeO2 nanorods) were tested in this reaction and their micromorphology and physical–chemical properties were characterized by transmission electron microscopy (TEM), X-ray diffraction (XRD), and N2 adsorption. CeO2 nanorods proved to be the most active catalytic material. The influence of different parameters on reaction outcome was studied. The yield of HDC was about 80% under optimized reaction conditions. Experiments for better understanding of reaction mechanism were also performed.
研究领域:
化学工程
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催化
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材料科学
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有机化学
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可持续化学
✓ 已验证
产品关联
DOI
高影响因子
Catalysis Science & Technology
·
2021
·Vol. 11
·期 13
·4581-4595
·
IF 6.119
Xuelong Lv,Songcai Cai,Jin Chen,Dongxu Yan,Mingzhu Jiang,Jing Chen,Hongpeng Jia
Enhancing the surface acidity has been seen as an effective strategy to optimize the performance of catalysts for the degradation of chlorinated volatile organic compounds (CVOCs). Herein, a series of catalysts are constructed by introducing Lewis and Brønsted acid sites into the skeleton surface of three-dimensional ordered macroporous (3DOM) CeO2. By a systematic study, we find that the introduction of Lewis acid sites can enhance the redox capacity of CeO2, while the surface Brønsted acid sites of the material promote chlorobenzene (CB) degradation through hydrolysis that is an effective degradation route to generate less chlorinated organic by-products. The optimal S–Ce0.7Zr0.3O2 with both abundant surface Lewis and Brønsted acid sites presents a stable activity and only 1.2% Cl2 selectivity with ∼90% CB conversion at 410 °C for 24 h. This work reveals the different roles and synergistic effects of Lewis and Brønsted acid sites to develop environmentally friendly CVOC combustion catalysts.
研究领域:
环境科学
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催化
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化学工程
·
污染控制
✓ 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）