Molecular Catalysis
·
2023
·
IF 4.6
Junya Cao,Xiaoxuan Wang,Liguo Wang,Yan Cao,Xiang Hui,Peng He,Huiquan Li
The carbonylation of 1,6-hexanediamine (HDA) is an important method for the production of dimethyl hexane-1,6-dicarbamate (HDC), which is of great significance for the non-phosgene synthesis of hexamethylene-diisocyanate. This research focuses on the synthesis of HDC through the methoxycarbonylation of HDA using methyl carbamate as a carbonyl source. The study investigates the utilization of CeO 2 catalyst prepared via H 2 O 2 assisted precipitation. Various characterization techniques, including N 2 physical adsorption and desorption, SEM, TEM, XRD, NH 3 TPD, CO 2 TPD, and XPS are employed to analyze the texture and structure of CeO 2 catalysts prepared through different methods. In situ FTIR experiments are conducted to monitor the potential process of the carbonylation reaction. The results of the in situ FTIR spectroscopy clearly indicate the formation of polyurea as an intermediate compound, which subsequently converts into HDC. The findings demonstrate that CeO 2 prepared using the hydrogen peroxide precipitation method exhibits a larger specific surface area, stronger acid-base properties, and a higher content of surface-adsorbed oxygen. These characteristics are favorable for the carbonylation reaction. Under optimized conditions, the HDC yield reaches 96.0% with complete conversion of HDA. The catalyst's activity essentially maintained throughout ten cycles. Additionally, a substrate versatility study reveals that CeO 2 exhibits excellent catalytic properties for synthesizing a range of aliphatic and alicyclic dicarbamates.
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COMPOSITES PART B-ENGINEERING
·
2023
·
IF 13.1
Zhiyao Chu,Junqi Li,Hong Yong Sohn,Chaoyi Chen,Xiao Huang,Yuanpei Lan,Arun Murali,Junshan Zhang
In this work, novel CeO 2 –C-g-C 3 N 4 S-scheme heterojunctions with significantly enhanced photocatalytic performance were prepared for the first time by a facile one-step molten KCl–LiCl method. The formation mechanism of CeO 2 –C-g-C 3 N 4 was discussed, where g-C 3 N 4 turned to C by carbonizing and the surface C content was adjusted by controlling the synthesis conditions. The photocatalytic property of the ternary composites first increased and then decreased with synthesis temperature and time. The 580 °C 4h CeO 2 –C-g-C 3 N 4 exhibited the best performance towards MB (Methylene blue) and TC (Tetracyclines) degradation with a removal degree of 99.9% and 92.5%, respectively. The surface C/N ratio was a key index that influenced the photocatalytic performance, and was calculated to be 0.918–1.352 for various CeO 2 –C-g-C 3 N 4 catalysts. The 580 °C 4h CeO 2 –C-g-C 3 N 4 had an appropriate C/N ratio of 0.930 and a narrow band gap. The formed S-scheme 2D heterojunctions and generated C clearly promoted the separation of photo-excited e - / h + . Besides, it was indicated that e - and · O 2 − were the main active species for TC photodegradation . The 580 °C 4h CeO 2 –C-g-C 3 N 4 exhibited a large BET surface area, high negative zeta potential , strong π-π electron donor-acceptor interaction, and an excellent MB adsorption ability. It was evident that chemisorption on catalyst surface played an important role for adsorbing MB. The formation mechanism of CeO 2 –C-g-C 3 N 4 and the effects of the surface C/N ratio on photocatalytic performance, determined in this work, offer new insights for preparing and structuring highly effective photocatalysts , which is expected to promote further photocatalytic and adsorption applications.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Peiyun Zhou,Guangtong Hai,Gongchi Zhao,Rushuo Li,Xiubing Huang,Yunfeng Lu,Ge Wang
Developing multifunctional electrocatalysts with excellent hydrogen evolution reaction (HER), oxygen evolution reaction (OER) and 5-hydroxymethylfurfural oxidation reaction (HMFOR) activities will contribute to "carbon neutrality". Here, CeO 2 is introduced into the Co 4 N system as an "electron pump" to attract electrons to transfer from Co 4 N to CeO 2 . The interface electronic structure optimization enables Co 4 N@CeO 2 to exhibit excellent HER, OER, and HMFOR performance. Specifically, to deliver 10 mA cm −2 current density, (1) it only requires low overpotentials of 49 and 263 mV for HER and OER in 1.0 M KOH, respectively; (2) it merely needs an ultra-low potential of 1.22 V RHE for HMFOR in 1.0 M KOH + 300 mM HMF, which is 273 mV lower than the required potential in 1.0 M KOH. Theoretical calculation results show that the introduction of CeO 2 effectively reduces the barriers for potential-determining steps of HER and OER, and optimizes OH - adsorption to promote the HMFOR process.
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FUEL
·
2022
·
IF 8.035
Xiaodi Li,Shan Ren,Lian Liu,Xiangdong Xing,Lin Chen,Jiangling Li,Jian Yang,Qingcai Liu
The serious deactivation of denitration catalysts caused by heavy metals still a thorny issue in the practical application of selective catalytic reduction of NO x with NH 3 . Herein, we proposed a novel anti-poisoning strategy by designing SO 4 2− /ZrO 2 superacid supported CeO 2 /ZrO 2 catalyst, and the effect of SO 4 2− /ZrO 2 supported CeO 2 /ZrO 2 for PbO-resistance NO x catalytic reduction was investigated. It was worthy to note that the introduction of solid superacid SO 4 2− /ZrO 2 significantly enhanced catalytic performance over the entire temperature range, with an exceptionally high NO x removal efficiency over 98 % during 250–500 °C. When 2 wt% PbO was deposited on the fresh catalyst, the catalytic activity of CeO 2 /ZrO 2 catalyst decreased obviously, while CeO 2 /ZrO 2 -S catalyst can still maintain a higher NO x conversion over 90 % from 275 to 500 °C. The characterization results confirmed that the introduction of solid superacid SO 4 2− /ZrO 2 enhanced the surface acidity and promoted the transformation from Ce 4+ to Ce 3+ . The results of in situ DRIFTS implied that the Eley-Rideal (E-R) mechanism was obeyed over CeO 2 /ZrO 2 catalyst, and both Eley-Rideal (E-R) and Langmuir-Hinshelwood (L-H) mechanisms were followed over CeO 2 /ZrO 2 -S catalyst in the SCR process. With regard to poisoned catalysts, the NH 3 adsorption was inhibited to some extent, while the reaction mechanism wasn’t changed by PbO poisoning.
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JOURNAL OF RARE EARTHS
·
2022
·
IF 4.632
Deyang Ning,Junqi Li,Yuanpei Lan,Hong Yong Sohn,Jian Yang,Chaoyi Chen,Zhiyao Chu,Xisong Mao
In this work, we firstly synthesized a CeO 2 /C 3 N 4 photocatalyst with Z-scheme heterojunction by a facile LiCl–KCl molten salt method. The synthesized catalyst has an excellent quality for removing organic pollution of dyes and antibiotics in wastewater. As an example, the CeCN–1:5 prepared with a mass ratio of Ce 2 (CO 3 ) 3 · x H 2 O:C 3 H 3 N 6 = 1:5 exhibits a methylene blue (MB) removal capacity of 100% within 90 min and tetracycline (TC) removal capacity of 94.6%. After 4 cycles, the CeCN–1:5 keeps a removal efficiency of nearly 100% in 150 min for MB and 85.7% for TC. The kinetics study reveals that the MB removal process with the CeCN–1:5 fits the modified Elovich model with strong adsorption while TC removal fits the first-order model. The large surface area (238 m 2 /g) and negative zeta potential (−39.3 mV) of CeCN–1:5 contribute to superior adsorption capacity to MB. However, the adsorption of TC is restricted due to the positive surface/pore potential in acidic solution. CeCN–1:5 has combined Z-scheme heterojunction and exhibits a low recombination rate of electrons (e – )/holes (h + ) and the photo-generated active radicals of · OH/ · O 2 – that promotes the photocatalytic performance. This novel CeO 2 /C 3 N 4 photocatalyst with an excellent photocatalysis removal activity has an enormous potential for photocatalytic applications.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Wei Liu,Hui Sheng,Liu Zhu,Yiwen Zhang,Wenxu Liu,Yuwei Zhao,Qian Li,Yong Peng,Zhongpeng Wang
The classical strong metal-support interaction (SMSI) plays a key role in improving thermal stability for supported Au catalysts. However, it always decreases the catalytic activity because of the encapsulation of Au species by support. Herein, we demonstrate that Al 3+ is a functional additive which could effectively improve both catalytic activity and sintering resistant property for H 2 pretreated Al 3+ doped CeO 2 supported Au (AuCeAl) catalyst at high temperature. The physical characterization and in-situ DRIFTS results provide insight that more oxygen vacancies generated by Al 3+ doping could be as preferential adsorption sites for CO molecules when the encapsulation of Au species occurred, which is certificated by an accelerated formation of bicarbonate species. In the meantime, smaller Au nanoparticles with higher dispersion (2.8 nm, 85.63%) is achieved in AuCeAl catalysts, compared with that in CeO 2 supported Au (AuCe) catalysts (5.1 nm, 36.17%). Additionally, the as-prepared AuCeAl catalysts also have superior catalytic performance even after calcination at 800 °C in air.
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CHEMICAL RESEARCH IN CHINESE UNIVERSITIES
·
2022
·Vol. 38
·期 6
·1547-1552
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IF 2.726
Jin Huan,Xu Ding,Tian Chao,Yue Yinghong,Hua Weiming,Gao Zi
A series of Sm-doped CeO 2 /Beta composite catalysts with various Sm/Ce atomic ratios(0.1–0.4) were prepared by an incipient impregnation method, followed by calcination at 650 °C. They were characterized by X-ray diffraction(XRD), N 2 adsorption, X-ray photoelectron spectroscopy(XPS), Raman, NH 3 -temperature programmed desorption(TPD) and CO 2 -TPD. The incorporation of Sm into CeO 2 /Beta increases obviously the propylene yield for the selective conversion of ethanol to propylene. The promoting effect of Sm on CeO 2 /Beta can be attributed to two reasons. One is more acetone intermediates are generated on the Sm-doped catalysts due to the enhanced formation of oxygen vacancies. The other is the conversion of acetone intermediate to propylene is enhanced owing to weaker and fewer acid sites on the Sm-doped catalysts.
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CERAMICS INTERNATIONAL
·
2025
·Vol. 51
·期 11
·14746-14754
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IF 5.6
Boyu Chen,Lijuan Niu,Jianlong Chai,Zhiyuan Bai,Jiayin Zhang,Di Liu,Xuefeng Lu,Yabin Zhu
β-SiC ceramics were prepared by spark plasma sintering at 2200 °C with Y 2 O 3 , MgO , and CeO 2 as sintering additives. Al 2 O 3 was doped based on the above oxides to form a two-component sintering additive to carry out a comparative analysis. The effects of these additives on the microstructure, bulk density, and Vickers hardness of β-SiC were systematically studied. The mechanical properties of the single-component samples were superior to those of the two-component samples. Notably, the single-component sample with Y 2 O 3 , addition exhibited the highest density (98.69 %) and hardness (27.1 GPa), which can be attributed to the appropriate growth of the grains in the single-component sample with Y 2 O 3 . Additionally, the principle of lattice reduction in SiC ceramics was explored using first-principle calculations, further highlighting the advantage of Y 2 O 3 as a single additive for the high-temperature sintering of SiC ceramics.
研究领域:
材料科学
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陶瓷学
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力学性能
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计算材料学
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-12
·
IF 15.7
Xu Feiyan,Zhao Feifan,Deng Xianyu,Zhang Jinfeng,Zhang Jianjun,Ai Chenbin,Yu Jiaguo,García Hermenegildo
The rapid increase in atmospheric CO 2 levels due to industrialization underscores the urgent need for innovative carbon valorization strategies. Photocatalytic CO 2 reduction presents a sustainable solution; however, conventional systems suffer from inefficient charge separation and limited product applicability. Herein, a green and scalable tandem strategy is developed by integrating S-scheme photocatalysis with palladium-catalyzed carbonylation. A rationally designed CeO 2 /Bi 2 S 3 heterojunction leverages its hierarchical structure, broad visible-light absorption, oxygen-vacancy-mediated charge dynamics, and the S-scheme charge transfer mechanism to achieve highly efficient photocatalytic CO 2 -to-CO conversion (14.05 mmol g −1 , 98% selectivity). The generated CO is directly utilized in a subsequent carbonylation reaction under mild conditions, yielding high-value amides with near-quantitative CO utilization. This integrated approach eliminates the risks of CO handling and enhances economic viability, providing a direct and effective route for converting CO 2 into fine chemicals. By bridging photocatalysis with industrial catalysis, this work advances sustainable carbon recycling technologies and opens avenues for the development of efficient CO 2 conversion systems.
研究领域:
环境科学
·
催化
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材料科学
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化学工程
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绿色化学
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Catalysts
·
2025
·Vol. 15
·期 9
·812
·
IF 4
Xinru Gao,Han Meng,Changan Wang,Jinzhang Tao,Hongyi Gao
The development of highly efficient catalysts for the hydrogenation of dicyclopentadiene (DCPD) remains a critical challenge. In this study, we designed a series of bimetallic Ce–Ni metal–organic framework (MOF)-derived nanocatalysts by precisely tuning the Ce/Ni ratio and calcination temperatures. The optimized catalyst, Ni–CeO2(7:3)@C–400 °C, featuring highly dispersed carbon-coated Ni nanoparticles, achieved complete hydrogenation of DCPD to tetrahydrodicyclopentadiene (THDCPD) with 100% conversion and nearly 100% selectivity within 2 h under 100 °C and 2 MPa. The porous carbon framework significantly facilitated the diffusion and accessibility of DCPD molecules, combined with Ce species reconstructing the electronic structure of Ni active centers through electronic interactions, synergistically enhancing the hydrogenation efficiency. Furthermore, the catalyst demonstrated good structural stability. This work not only provides a robust strategy for the rational design of bimetallic MOF-derived catalysts but also highlights their potential for practical applications in industrial hydrogenation processes.
研究领域:
催化化学
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材料科学
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加氢化学
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纳米材料
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金属有机框架（MOFs）
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 29
·期 23
·34861-34873
·
IF 5.19
Humayun Muhammad,Shu Lang,Pi Wenbo,Xia Hui,Khan Abbas,Zheng Zhiping,Fu Qiuyun,Tian Yahui,Luo Wei
The design of highly efficient photoca talysts for clean energy production and environmental remediation are the grand challenges of scientific research. Herein, TiO 2 @MIL53Fe and CeO 2 @MIL53Fe composite photocatalysts are synthesized via solvothermal technique. The SEM and TEM micrographs reveal that TiO 2 and CeO 2 nanoparticles are vertically grown onto the surface of MIL53Fe MOF. Further, HRTEM micrograph confirmed the formation of heterojunction. It has been investigated that the resultant TiO 2 @MIL53Fe and CeO 2 @MIL53Fe photocatalysts exhibit remarkably improved visible light activities for H 2 production and 2,4-dichlorophenol (2,4-DCP) degradation in comparison to the bare MIL53Fe photocatalyst. The enhanced photoactivities of the fabricated TiO 2 @MIL53Fe and CeO 2 @MIL53Fe photocatalysts are attributed to significantly promoted charge separation as confirmed via the surface photo voltage (SPV) and photoluminescence (PL) results. Further, the photocatalysts exhibit high stability and reusability as confirmed via the recyclable tests. This work will promote the design of MOF-based efficient photocatalysts for clean energy production and environment purification.
研究领域:
材料科学
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环境科学
·
能源科学
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Advanced Healthcare Materials
·
2025
·
IF 9.6
Mei Zhou,Tingting Xu,Shengnan Yuan,Xuqiang Ma,Xue Yang,Jinbing Xie,Dehong Hu,Shenghong Ju
Triple-negative breast cancer (TNBC) is an aggressive subtype with rapid progression, high metastatic risk, and limited treatment options. Clinical TNBC specimens show severe hypoxia along with elevated expression of secreted protein acidic and rich in cysteine (SPARC). Inspired by these patient-derived hallmarks, it is engineered targeted self-assembled albumin-cerium oxide nanozymes (ACCD NPs) that couple SPARC-mediated tumor targeting with catalytic hypoxia modulation for synergistic sonodynamic-chemotherapy. Albumin enables selective delivery of doxorubicin (DOX) and chlorin e6 (Ce6) via SPARC-receptor interactions, while oxygen vacancy-engineered cerium oxide (CeO 2 ) decomposes endogenous hydrogen peroxide to generate oxygen, alleviating hypoxia. This oxygenation markedly amplifies ultrasound-triggered reactive oxygen species production, potentiating Ce6-mediated sonodynamic cytotoxicity and enhancing DOX chemosensitivity. In vitro, ACCD NPs demonstrate efficient targeted uptake, lysosome-responsive DOX release, and strong synergistic killing under ultrasound irradiation. In vivo, they achieve 3.8-fold higher tumor accumulation than free drugs, suppress TNBC growth by 84.9%, and downregulate hypoxia-inducible factor-1α (HIF-1α) without systemic toxicity. Mechanistic analyses reveal activation of autophagy and pyroptosis, suppression of oncogenic signaling, and upregulation of tumor suppressor genes. This clinically informed nanoplatform establishes a versatile therapeutic paradigm that translates patient tissue-derived molecular features into precise, multimodal strategies for overcoming hypoxia-associated, treatment-refractory cancers.
研究领域:
肿瘤学
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纳米医学
·
癌症治疗
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生物医学工程
·
活性氧信号传导
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