Nature Communications
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2024
·Vol. 15
·期 1
·1-10
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IF 14.7
Wang Hui,Cui Guoqing,Lu Hao,Li Zeyang,Wang Lei,Meng Hao,Li Jiong,Yan Hong,Yang Yusen,Wei Min
The dry reforming of methane provides an attractive route to convert greenhouse gases (CH 4 and CO 2 ) into valuable syngas, so as to resolve the carbon cycle and environmental issues. However, the development of high-performance catalysts remains a huge challenge. Herein, we report a 0.6% Ir/CeO 2− x catalyst with a metal-support interface structure which exhibits high CH 4 (~72%) and CO 2 (~82%) conversion and a CH 4 reaction rate of ~973 μmol CH4 g cat −1 s −1 which is stable over 100 h at 700 °C. The performance of the catalyst is close to the state-of-the-art in this area of research. A combination of in situ spectroscopic characterization and theoretical calculations highlight the importance of the interfacial structure as an intrinsic active center to facilitate the CH 4 dissociation (the rate-determining step) and the CH 2 * oxidation to CH 2 O* without coke formation, which accounts for the long-term stability. The catalyst in this work has a potential application prospect in the field of high-value utilization of carbon resources.
研究领域:
化学工程
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环境科学
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材料科学
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PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2021
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IF 5.316
Xisong Mao,Xuewen Xia,Junqi Li,Chaoyi Chen,Xiaoying Gu,Song Li,Yuan-Pei Lan
In this work, various new-observed structured CeCO 3 OH were synthesized by a self-assembly hydrothermal method , and a novel tactic to produce CeO 2- x with excellent photocatalytic activity by decomposing CeCO 3 OH in H 2 was proposed and identified. By controlling the synthetic conditions, almond-like, subglobose shape and hollow-sphere of CeCO 3 OH, 3D-broom-like of Ce 2 O 3 · 2CO 2 · nH 2 O (n = (1–2)), and sheet-like of Ce 2 (CO 3 ) 3 · 6H 2 O were synthesized. The crystal growth and formation of the cerium carbonate compounds were carefully studied using XRD , SEM and TEM. TG, thermodynamic calculation and in-situ XRD were employed to reveal the decomposition behavior of almond-like CeCO 3 OH in air, Ar and H 2 . The results show that the decomposition temperatures of CeCO 3 OH in Ar and H 2 are higher than that of in air, and suggest that Ce 2 O 3 has a low thermodynamic stability during the decomposition of CeCO 3 OH in Ar and H 2 , and Ce 3+ will be mostly oxidized by H 2 O firstly and then by both of H 2 O and CO 2 . The ceria samples obtained by decomposing from CeCO 3 OH in different atmosphere maintain indistinguishable shape and particle size. The XPS , Raman spectra and ESR results indicate that the one obtained in H 2 has the richest surface oxygen vacancies (OVs), narrowest band gap of 3.12 eV, lowest intensity in PL spectra and a significantly enhanced photodegradation ratio of methylene blue. The MB photodegradation ratio after 120 min reaction with the catalysts of CeO 2 -Air, CeO 2 -Ar and CeO 2 -H 2 is 43.14%, 54.43% and 73.41%, with a calculated reaction rate constant of 0.00539, 0.00652 and 0.01097 min -1 , respectively. The offered novel tactic of decomposing CeCO 3 OH in H 2 is an efficient and facile technique for active CeO 2- x production.
研究领域:
材料科学
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化学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Burenbayaer Borjigin,Lan Ding,Chenghong Liu,Huiqin Li,Xiaojing Wang
The exploration of highly efficient methods for degrading VOCs, with concurrent low energy consumption and lasting reusability, holds significant appeal. In this regard, an S-type CuBi 2 O 4 /CeO 2-x heterojunction with the robust interfacial interactions is presented as an active photocatalyst for the efficient decomposition of gaseous toluene under full-spectrum irradiation. The optimal sample CC15 effectively degrades gaseous toluene at a high concentration of 1800 ppm within 2 h, achieving a notable CO 2 yield of 87.05 %, and a TOC (total organic carbon) removal rate of 89.33 %. Furthermore, CuBi 2 O 4 /CeO 2-x exhibits exceptional stability, maintaining its 100 % degradation capability over 32 cycles for nearly 64 h. Comparative characterization reveals that the superior performance derives from an abundance of oxygen vacancies and effective pre-adsorption capabilities, which facilitate rapid adsorption of VOCs on the catalyst surface, thereby increasing the likelihood of degradation reactions. Additionally, the formation of an S-type heterojunction, valence pairing between Bi 3+ and Ce 3+/4+ ions, and strong interfacial interactions serve as the primary pathways for the efficient separation of photogenerated carriers, contributing to the high CO 2 production rate and prolonged cycle stability. The present investigation underscores the significant potential of vacancy-rich S-type heterojunctions and interfacial interactions between composite components, offering excellent activity and long-term availability for VOCs removal.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
LANGMUIR
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2022
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IF 4.331
Jinling Li,Hui-Ling Peng,Changchun Wen,Peijing Xu,Xing-Can Shen,Cunji Gao
The therapeutic effect of photothermal therapy (PTT) and photodynamic therapy (PDT) is severely limited because of the shallow tissue penetration depth of the first near-infrared (NIR-I) light. Multifunctional nanotheranostics irradiated by the second near-infrared (NIR-II) light have received wide interest with respect to deeper tissue penetration, and sonodynamic therapy (SDT) synergistic phototherapy can achieve the complete elimination of tumors. Herein, we successfully constructed a single NIR-II light-induced nanotheranostic using cerium oxide (CeO2–x) with abundant oxygen vacancies for photoacoustic imaging-guided SDT-enhanced phototherapy for the first time. CeO2–x with surface crystalline disorder showed extensive NIR-II region absorption and an outstanding photothermal conversion ability. In addition, the CeO2–x layer with numerous oxygen defects can promote the separation of holes and electrons by ultrasound irradiation, which can remarkably enhance the efficacy of phototherapy to achieve high-efficiency tumor ablation. CeO2–x was surface modified with hyaluronic acid (HA) to prepare CeO2–x@HA to allow active tumor targeting efficiency. Both cell and animal experiments confirmed that all-in-one CeO2–x@HA exhibited a high therapeutic efficacy of SDT-enhanced PDT/PTT under 1064 nm laser irradiation, which achieved complete tumor eradication without systemic toxicity. This study significantly broadened the application of NIR-II-responsive CeO2–x for photoacoustic imaging-mediated SDT-enhanced phototherapy to the highly efficient and precise elimination of tumors.
研究领域:
肿瘤学
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生物医学工程
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纳米医学
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Jiaxin He,Zhi-Hao Zhao,JinJin Li,Zhipeng Ren,Ruyi Jiang,Jichao Zhang,Jian Zhang
As pivotal high-performance elastomers, hydrogenated nitrile butadiene rubber (HNBR) was commonly manufactured by selective hydrogenation of nitrile butadiene rubber (NBR). Nevertheless, the high cost and poor stability of current noble metal-based catalysts seriously limit their large-scale applications. Herein, we report single-atom Pd supported by oxygen vacancies-rich CeO 2−x nanorods (Pd 1 /CeO 2−x ) as a novel catalyst for selectively hydrogenating the NBR. As a result of strong interaction between single-atom Pd and CeO 2−x support, the electrophilicity of Pd sites, and the nucleophilicity of olefinic bonds in NBR, the Pd 1 /CeO 2−x show a very high hydrogenated degree of 97.6 %, an unprecedentedly high Pd mass activity of 93.9 g NBR g Pd −1 h −1 , and outstanding cycling stability, which considerably outperform those for previously reported catalysts. Therefore, this work will promote the low-cost manufacture of HNBR and the exploration of single-atom catalysts for selective hydrogenation.
研究领域:
化学工程
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材料科学
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催化
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高影响因子
Molecular Catalysis
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2024
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IF 3.9
Yi He,Peng Bai,Shibo Yuan,Jiafa Chen,Yicheng Zhao,Yongdan Li
N -formylation of amines with CO 2 is a promising approach to high-efficient utilization of CO 2 as C1 feedstock, while conventional thermocatalytic processes suffer from harsh reaction condition and intense energy consumption. In this work, photocatalytic N -formylation of amines with CO 2 is achieved at room temperature over Pt-Bi/CeO 2− x composite catalyst. The Pt-Bi bimetallic sites increase the concentration of surface oxygen vacancies. Furthermore, the synergistic effects of Pt and Bi improve the light absorption capacity, reduce the band gap energy of the photocatalyst and promote the separation of photoinduced charge carriers. Using PhSiH 3 as the reducing agent, the conversion of N -methylaniline reaches 100 % after 3 h irradiation in N, N -dimethylformamide solvent with a N- methylformanilide selectivity of 90.8 %. The composite photocatalyst shows promising cycling stability and universality.
研究领域:
化学
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催化
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材料科学
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环境科学
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DOI
高影响因子
Journal of Materials Chemistry B
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2020
·Vol. 8
·期 37
·8634-8643
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IF 5.344
Yongmei Li,Yuemei Li,Yandong Bai,Laixiang Lin,Yina Sun
Cerium oxide nanoparticles (NPs) due to their advanced catalytic performance have been widely used to treat oxidative damage. However, Ce2O3 NPs have not been further investigated in the treatment of acute oxidative injury in vivo. It is meaningful to improve the efficiency for treatment of acute oxidative injury with NPs in vivo. In this report, we designed Er3+-doped Ce2O3 (Er/Ce2O3) NPs with a size of 7.9 nm, which were used to treat acute liver injury. Er/Ce2O3 NPs realized high-efficiency catalysis of hydrogen peroxide (H2O2) at room temperature. An acute liver damage model was established through intraperitoneal injection of lipopolysaccharide (LPS) in C57 mice. By analyzing histopathological and biochemical indexes, Er/Ce2O3 NPs showed a significant improvement in LPS-induced acute liver injury. Acute liver oxidative damage can be treated within 24 hours, which proved the high catalytic efficiency of Er/Ce2O3 NPs in vivo. The activities of SOD, GPx and CTA increased and production of ROS decreased with Er/Ce2O3 NP treatment in comparison with LPS-induced injury, indicating that the mechanism of Er/Ce2O3 NPs in the treatment of acute oxidative damage of liver was mainly via catalysis of ROS products. Moreover, the protein expression levels of TNF-α, CD45 and IL-1β in liver decreased in the Er/Ce2O3 NPs-treated group, which indicated that Er/Ce2O3 NPs have the function of anti-inflammation property. Therefore, Er/Ce2O3 NPs can be applied to treat and prevent diseases caused by acute oxidative damage.
研究领域:
纳米技术
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生物医学工程
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药理学
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毒理学
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DOI
PubMed
高影响因子
OPTICAL MATERIALS
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2022
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IF 3.754
Cheng Zuo,Xishi Tai,Qian Su
S-scheme heterojunction can accelerate the separation of photogenerated electron-hole pairs and retain strong redox ability, so it has outstanding advantages and application prospects in the field of photocatalysis . The Ce 3+ self-doping CeO 2-x @CuO nanowires arrays on copper mesh were synthesized with the strategy of surface hydrogenation and hydrothermal calcination method. The morphology, composition and properties of the catalysts were determined by SEM, TEM, EDS , UV-VIS, PL , CO 2 -TPD and other characterization methods. Ce 3+ self-doping introduces O vacancies on the surface of CeO 2 without introducing heteroatoms. The O vacancies of CeO 2-x could enhance the adsorption, activation and reduction of CO 2 . The existence of coaxial S-scheme heterojunctions could effectively enhance the light absorption range and the separation of photo-generated charges. The photocatalytic activity of the composite catalyst was much higher than that of pure CuO/copper mesh (CM) and CeO 2 , and the difference in activity of catalysts composed of different proportions was studied. When the Ce 3+ self-doping CeO 2-x loading was moderate, the methanol yield reached 6.73 μmol·g cat −1 after 4 h reaction under visible light , which is 5.26 times of CuO/CM and 9.35 times of CeO 2 . The reduction mechanism of the composite catalyst at the gas-liquid interface was studied. This work demonstrates a feasible strategy to create efficient S-scheme heterojunction photocatalysts with rich active surface O vacancies for photocatalytic CO 2 reduction.
研究领域:
材料科学
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环境科学
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光催化领域
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DOI
高影响因子
CHINESE JOURNAL OF STRUCTURAL CHEMISTRY
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2026
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IF 10.5
Ju-Hua Li,Yong Tian,Jia-Yi Chen,Hong-Kai Guo,Wen-Hao Wang,Yu-Shu Han,He-Xuan Zhang,Xiao-Yu Zhang,Zhong-Li Wang
Citric acid adsorbed CeO 2 forms a uniformly dispersed nanoparticle sol, acting as a special “glue” to uniformly adhere to the surface of the NiMoO 4 precursor. • Under high-temperature reduction, a CeO 2-x modified NiMo alloy with strong interaction is synthesized. • The optimized composite electrocatalyst achieves an overpotential of only 48 mV at 10 mA cm -2 with the stability for over 1,500 h at 500 mA cm -2 . • In situ Raman spectra and DFT calculations indicate that the CeO 2-x /NiMo alloy interface accelerates water dissociation and enhances alkaline HER performance. NiMo alloys are promising non-precious metal electrocatalysts for alkaline hydrogen evolution reaction (HER), however, they suffer from issues such as poor stability due to Mo leaching and insufficient intrinsic activity. In this study, a citric acid (CA) assisted CeO 2-x modification strategy is developed to prepare a CeO 2-x /NiMo alloy composite electrocatalyst with high activity and stability. CA is uniformly adsorbed onto the surface of CeO 2 nanoparticles, and the cross-linked CA network with the CeO 2 particles forms a uniformly dispersed nanoparticle sol, which acts as a special “glue” to uniformly adhere to the surface of the NiMoO 4 precursor, forming a CeO 2 /NiMoO 4 composite precursor. Following high-temperature reduction, a CeO 2-x modified NiMo alloy electrocatalyst is synthesized. Owing to the strong interaction between CeO 2-x and NiMo, the optimized composite electrocatalyst achieves a current density of 10 mA cm -2 at an overpotential of only 48 mV and it maintains high stability for over 1500 h at a current density of 500 mA cm -2 , which is three times longer than that of the unmodified NiMo alloy electrocatalyst, outperforming most reported nickel-molybdenum-based electrocatalysts. In situ Raman spectra and density functional theory calculations indicate that the CeO 2-x /NiMo alloy interface accelerates water dissociation, hydrogen combination and enhances alkaline HER performance. This work provides a new approach for the preparation of highly active and stable nickel-molybdenum-based hydrogen evolution catalysts. A citric acid assisted CeO 2-x modification strategy is developed to prepare a highly-active and stabile CeO 2-x /NiMo alloy electrocatalyst for HER. Download: Download high-res image (267KB) Download: Download full-size image
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DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2025
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IF 6.3
Yin Liu,Liang Shuai,Lei Cao,Qian Zhu,Lanlan Fan,Liang Xu,Shixian Xiong
The widespread use of carbendazim (CBZ) fungicide calls for monitoring its toxic residues in food due to human health concerns. Herein, a Ru/CeO 2-x heterostructured composite was constructed by sodium borohydride reduction for the electrochemical sensing of CBZ. The rational design engineers abundant interfacial oxygen vacancies and Ru nanoclusters, which form interfacial Lewis acid-base pairs capable of dual-site recognition of CBZ molecules. Specifically, oxygen-vacancy Lewis acidic sites preferentially adsorb the electron-rich groups(such as lone pairs on amino groups), while Ru-based Lewis basic sites capture electron-deficient carbon atoms within the benzimidazole ring. Such synergistic adsorption and interfacial charge transfer markedly enhance the redox kinetics of CBZ. Consequently, the Ru/CeO 2-x /GCE sensor delivers an ultralow detection limit of 7.7 nM, along with excellent selectivity, reproducibility, and long-term stability. This work provides a new interfacial engineering strategy integrating oxygen-defect chemistry and electronic modulation for designing high-performance Lewis acid–base coupled sensing materials.
研究领域:
环境监测
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电分析化学
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纳米材料
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传感材料
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食品安全
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Xingyu Zhang,Chenliang Zhou,Shaoyuan Shi,Xuequan Jing,Zhi Zheng,Wenjing Yuan
Building narrow band gap semiconductors and fast separation of photogenerated electron-hole (e - -h + ) structures are of great significance for photocatalytic process. In this contribution, the CeO 2-x /C 3-y N 4 /Ce(CO 3 )(OH) double S-scheme heterojunctions with atomic vacancies tunable band gap (2.54 eV) have been designed and fabricated as a boost photocatalyst for enrofloxacin (ENR) photodegradation. Compared with the control samples, the experimental results indicate that the typical sample (CeO 2-x /C 3-y N 4 /Ce(CO 3 )(OH)-2) achieves the highest ENR photodegradation efficiency (93.6 %) in 240 min under a pH of 6, and the possible photodegradation pathways are also proposed. The superior performance is ascribed to the CeO 2-x /C 3-y N 4 /Ce(CO 3 )(OH) double S-scheme heterojunctions for selective recombination of photogenerated electrons with weak-reduction ability in conduction band (CB) of CeO 2-x , C 3-y N 4 and the photogenerated holes with weak-oxidation nature in valance band (VB) of C 3-y N 4 , Ce(CO 3 )(OH), which increase the retention rate of photogenerated electrons in CB of Ce(CO 3 )(OH) and photogenerated holes in VB of CeO 2-x to degrade ENR. This is the first systematic study of CeO 2-x /C 3-y N 4 /Ce(CO 3 )(OH) double S-scheme heterojunctions for ENR photodegradation.
研究领域:
环境科学
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材料科学
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产品关联
DOI
PubMed
高影响因子
Green Chemical Engineering
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2026
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IF 11.9
Jiaxin He,Shangqi Zhou,Lisha Guo,Siying An,Rui Bai,Wenxiu Ma,Jin Lin,Jichao Zhang,Menglei Yuan,Jian Zhang
Palladium single-atom catalysts show exceptional catalytic performance in nitrile butadiene rubber (NBR) hydrogenation due to their unique unsaturated coordination environments. However, the hydrogenation activity and atomic efficiency are seriously limited by inherent instability of undercoordinated Pd δ+ sites and poor support structure, leading to decreased hydrogenation degree and cycling stability. In this work, a novel single-atom palladium catalysts was developed, where undercoordinated single-atom Pd δ+ sites are steadily anchored onto CeO 2- x nano-islands supported by SiO 2 (Pd 1 /CeO 2- x /SiO 2 ). The strong metal-interaction of CeO 2- x nano-islands immobilize the undercoordinated Pd δ+ sites to enhance adsorption of olefin bonds in NBR, while SiO 2 promotes mass transfer diffusion of NBR and atomic efficiency of palladium. The Pd 1 /CeO 2- x /SiO 2 thus achieves an unprecedented hydrogenation degree of up to 99.8% without decrease over a 10-runs stability test in selective hydrogenation of NBR, outperforming previously state-of-the-art catalysts. Consequently, this work will offer a new strategy for single-atom catalysts to achieve high steady-state activity in selective hydrogenation.
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高影响因子
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