CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Xuyi Tao,Xu Wang,Chunzi Yang,Ming Zhao,Chao Wang,Chunmei Zhang,Jixue Lu,Shan Zhang,Ruguang Ma,Chunxian Guo
Urea-assisted water splitting that involves urea oxidation reaction (UOR) and hydrogen evolution reaction (HER) can purify urea-rich wastewater and produce hydrogen, but the lack of efficient catalysts hampers its application. Ni(OH) 2 is recognized as one of the most active electrocatalysts for UOR but the performance is hindered by the limited active sites with intrinsic activity. Herein, porous Ni(OH) 2 nanosheets with Ce and N codoping (Ce, N Ni (OH) 2 ) are designed to regulate electrochemical microenvironment and used as a bifunctional catalyst for urea-assisted water splitting. The porous structure enhances the exposure of rich active sites, while the Ce, N-codoping optimizes the d band center of active Ni species and improves electron transport. In-situ Raman spectroscopy and theoretical calculation disclose the real active sites are γ-NiOOH species generated during the UOR process and the regulated microenvironment promotes a shift in the rate-controlling step of the UOR from CONNH* dehydrogenation to CONHNH* dehydrogenation with a reduced thermodynamic barrier. As a result, the Ce, N-Ni(OH)₂ catalyst delivers excellent UOR activity with a low potential of 1.39 V at 100 mA cm −2 and a small Tafel slope of 18.4 mV dec −1 , along with superior HER activity. The assembled urea-assisted electrolyzer achieves a low cell voltage of 1.49 V at 10 mA cm −2 and maintains robust operational stability over 70 h. This work demonstrates a synergistic design strategy of porous structure and dual-element modulation, offering a new avenue for developing advanced catalysts in sustainable energy and environmental applications.
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
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2022
·Vol. 33
·期 16
·13271-13289
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IF 2.779
Yu Xiaochen,Song Zeyu,Dong Xiaoqian,Li Huajian,Liu Haonan,Zhao Baoyan,Ye Ting,Jiang Yinlin,Li Xiaojie,Duan Li,Fan Jibin,Zhao Peng
g-C 3 N 4 and rare earth (RE)-doped (Yb, Nd and Ce) g-C 3 N 4 nanosheets were synthesized by a thermal method. The remarkable effects of RE doping on the structural, morphological, and optical properties of g-C 3 N 4 were investigated using XRD, FT-IR, SEM, BET, XPS, UV–Vis, PL, EIS and Mott–Schottky characterization techniques. The photocatalytic activities of RE doped g-C 3 N 4 nanosheets for different dyes were improved compared with g-C 3 N 4 under visible light irradiation, among which Ce/g-C 3 N 4 showed outstanding performance. Due to the doping of RE, it modulates the electronic structure of pristine g-C 3 N 4 and broadens its optical absorption range. In addition, a possible mechanism of photocatalytic degradation of dyes was propounded by free radical trapping experiments. This work may provide a reference for the rational design of photocatalysts and inspiration for the photocatalytic mechanism.
研究领域:
材料科学
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环境科学
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化学
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2026
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IF 19.7
Siyu Wu,Zining Qiu,Yuan Zhang,Xiaoya Zhao,Mingchen Zhou,Le Zhang,Cheng-Peng Li,Zhenhua Yan,Hongming Sun
Construct PtCu/CeO 2 heterojunction to resolve alkaline HER activity-stability trade-off dilemma. • Form strong Pt-O-Ce interfacial bonds to restrain Pt oxidation and metal leaching. • CeO 2 serves as efficient promoter to drastically accelerate water dissociation step of alkaline HER. • Assembled AEMWE cell delivers 2500 h ultra-long stability at industrial current density. The persistent activity-stability trade-off in electrocatalysts, driven by the dynamic evolution of active sites, severely limits the practical application of anion exchange membrane water electrolysis (AEMWE). Herein, we construct a robust PtCu/CeO 2 heterostructure that simultaneously achieves superior activity and long-term durability for alkaline hydrogen evolution reaction (HER). The catalyst exhibits an ultralow overpotential of 10 mV at 10 mA cm −2 and a small Tafel slope of 23.2 mV dec −1 , significantly outperforming conventional Pt/Ni(OH) 2 and Pt/C electrodes. In a full AEMWE cell, the PtCu/CeO 2 ||NiFe LDH system requires only 1.71 V to reach 1 A cm −2 and maintains stable operation for 2500 h with negligible decay, ranking it among the best-performing alkaline HER catalysts. Mechanistically, Cu alloying optimizes the hydrogen adsorption energy of Pt, while CeO 2 acts as an effective water dissociation promoter to accelerate the overall reaction kinetics. Moreover, strong Pt-O-Ce interfacial bonding between the thermodynamically stable CeO 2 and PtCu alloy, together with significant hybridization of Pt 5d/Cu 3d and Ce 4 f/O 2p orbitals, effectively suppresses the dissolution and oxidation of Pt sites. thereby enhancing the durability of the catalyst under high-current-density operation. This work offers a viable strategy to overcome the activity-stability dilemma in HER catalysts for industrial AEMWE. Download: Download high-res image (142KB) Download: Download full-size image This work presents a robust PtCu/CeO 2 heterostructure that breaks the activity-stability trade-off in alkaline HER for AEMWE. CeO 2 acts as an efficient water dissociation promoter, accelerating the Volmer step. It also serves as a thermodynamically stable scaffold. Strong Pt-O-Ce interfacial bonding optimizes the electronic structure and suppresses Pt dissolution and oxidation. This catalyst achieves superior activity with an overpotential of 10 mV at 10 mA cm −2 . In a full AEMWE cell, it demonstrates stable operation for 2500 h at 1 A cm −2 .
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
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IF 5.2
Dongsheng Chen,Xiangyang Xu,Pengtao Lei,Jianyu Ge,Yuanlin Tong,Chenyu Huang,Xianghui Fu
Morphology control and heterostructure construction are two essential aspects in designing and synthesizing photocatalysts . Herein, hollow microsphere heterojunctions of CeO 2 and Ce 3+ doped BiOBr (Ce-BiOBr) were fabricated adopting a facile one-pot solvothermal approach. Owing to the positively charged Ce species, the interlamellar repulsion can be reduced and the specific surface area of these microsphere can be increased. The as-generated Ce 4+ /Ce 3+ redox centers can synergistically improve the transfer and separation efficiency of photogenerated carriers. When used to treat Congo red (CR), 0.1CBOB with a Ce/Bi molar ratio of 0.1:1 exhibits the best photodegradation efficiency (94.63%) and kinetic rate (0.01119 min −1 ) under visible light-emitting diode (LED) light irradiation , which are remarkably superior to pure BiOBr and CeO 2 . The results of radical capture experiment show that photogenerated hole (h + ), superoxide radical (·O 2 − ) are the main active species in the process of photocatalytic degradation.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Lan Ding,Fenghua Bai,Burenbayaer Borjigin,Yuning Li,Huiqin Li,Xiaojing Wang
Solar-energy-driven CO 2 conversion into valuable chemical fuels holds great renewable potential. However, most photocatalysts' weak CO 2 adsorption limits more artificial photosynthesis for further utilization. Herein, we present an in situ assembling approach to produce stable Cs 2 AgBiBr 6 /Ce-UiO-66-H composite, in which a tight contact interface between the two participated components was constructed. Benefiting from the photocatalytic properties and high adsorption capacity for CO 2 , the optimized 20Cs 2 AgBiBr 6 /Ce-UiO-66-H adsorption-photocatalyst exhibits outstanding performance for reductive CO 2 deoxygenation with considerable CO generation rate (309.01 μmol g −1 h −1 ) under simulated solar light irradiation with 300 W Xe lamp, which is about 2.1 and 2.7 times than that of pure Cs 2 AgBiBr 6 and Ce-UiO-66-H, respectively. The excellent catalytic conversion of CO 2 is ascribed to the effective solar harvest and quickly photo-excited carriers’ separation in such assembled architecture. Importantly, due to the in-situ synthesis, Cs 2 AgBiBr 6 QDs are intercalated in the Ce-UiO-66-H frameworks and it could lead to improved stability and induce abundant oxygen vacancies in Cs 2 AgBiBr 6 /Ce-UiO-66-H, which can maintain unchangeable CO 2 conversion rate under wet air with consecutive ten hours of the recycling test. In this work, the combining metal–organic frameworks and lead-free halide perovskite provide great potential for artificial photocatalytic CO 2 -to-CO conversion under a mild gas–solid reaction condition via utilizing solar energy.
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ACS Applied Materials & Interfaces
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2022
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IF 10.383
Jiejun Ren,Andries Meijerink,Xiaopeng Zhou,Jiapeng Wu,Gangyi Zhang,Yuhua Wang
All-inorganic perovskite quantum dots (PQDs), which possess outstanding photophysical properties, are regarded as promising materials for optoelectronic applications. However, the poor light conversion efficiency and severe stability problem hinder their widespread applications. In this work, a novel encapsulation strategy is developed through the in situ growth of CsPbX3 PQDs in presynthesized mesoporous cerium-based metal organic frameworks (Ce-MOFs) and further silane hydrolysis–encapsulation, generating stable CsPbX3@Ce-MOF@SiO2 composites with greatly enhanced light conversion efficiency. Moreover, the simulation results suggest that the pore boundary of Ce-MOFs has a strong waveguide effect on the incident PQD light, constraining PQD light inside the bodies of Ce-MOFs and suppressing reabsorption losses, thus increasing the overall light conversion efficiency of PQDs. Meanwhile, the Ce-MOF@SiO2 protective shell effectively improves the stability by blocking internally embedded PQDs from the harmful external environment. Further, the obtained white-light-emitting diode shows an ultrahigh luminous efficiency of 87.8 lm/W, which demonstrates their great potential in optoelectronic applications.
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PubMed
高影响因子
MICROCHEMICAL JOURNAL
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2023
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IF 4.8
Xuemei Wang,Yuan Ma,Zheng Zhou,Zhen Zhang,Jie Zhang,Lin Fan,Xinzhen Du,Xiaoquan Lu
Simple and rapid analytical methods for pharmaceuticals and personal care products (PPCPs) are in high demand for environment monitoring. Herein, an in-situ doping strategy was used to ultrarapid synthesize carbon black (CB)-doped Ce (III, IV)-MOF composite with dumbbell-shaped structure at room temperature, which had been used as an electrochemical sensor for the effective and simultaneous detection of typical PPCPs such as dopamine (DA) and acetaminophen (AC) in complex matrices samples using different pulse voltammetry (DPV). Scanning electron microscope (SEM), Nitrogen adsorption-desorption, X-ray photoelectron spectroscopy (XPS), Fourier transform infrared spectroscopy (FT-IR), and X-ray powder diffractometer (XRD) were used to characterize the morphological and electrochemical properties of synthesized a series material. The mixed-valent CB/Ce (III, IV)-MOF with excellent pore structure properties provided more exposed active sites, which were more conducive to adsorption and thus improved sensing performance. The result showed that the proposed method had a wide linear range (for DA: 0.3–252.0 µM, for AC: 0.3–252.0 µM) and low detection limits (for DA: 0.0955 µM, for AC: 0.1170 µM). Based on the synergistic effect of both CB and Ce (III, IV)-MOF, the composites modified electrodes had excellent electroanalytical capability for DA and AC, which could be used for efficient and rapid monitoring of ECs and the construction of new electrochemical sensor based on MOFs.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Huijiao Wang,Zhongyi Li,Fengyuan Zhang,Yuxiang Wang,Xian Zhang,Jianbing Wang,Xuwen He
Three types of Magnéli phase anodes (Ti/Ti 4 O 7 , Ti/Ti 4 O 7 -PbO 2 -Ce, and Ti/Ti 4 O 7 nanotube arrays (NTA)) were fabricated, characterized, and compared with other typical active and non-active anodes (i.e., BDD, Ti/Pt, Ti/RuO 2 -IrO 2 , and Ti/IrO 2 -Ta 2 O 5 ) for electro-oxidation treatment of p -nitrophenol (PNP) solution and a real coal chemical concentrated brine in this study. Characterization results indicate a nanotube array structure of Ti/Ti 4 O 7 NTA, and a compact coating of Ti 4 O 7 microparticles and PbO 2 -Ce nanocrystals on the Ti substrate for Ti/Ti 4 O 7 and Ti/Ti 4 O 7 -PbO 2 -Ce, respectively. The three anodes present relatively high oxygen evolution potentials (2.16–2.44 V vs SCE), showing good capacity of electro-generating reactive oxidative species for pollutant degradation. After 30 min of EO treatment, Ti/Ti 4 O 7 NTA and Ti/Ti 4 O 7 removed 89–92% of PNP, which were 10–60% higher than Ti/Pt, Ti/RuO 2 -IrO 2 , and Ti/IrO 2 -Ta 2 O 5 , and were almost comparable with BDD (95%). Furthermore, Ti/Ti 4 O 7 NTA and Ti/Ti 4 O 7 kept very efficient for mineralization of PNP solution and real coal chemical concentrated brine. For Ti/Ti 4 O 7 -PbO 2 -Ce, its degradation efficiency was lower than other two Magnéli phase anodes, but still competitive compared with other active anodes. Thanks to their high removal efficiencies, the three Magnéli phase anodes required relatively low energy demand for pollutant mineralization. Besides, operational parameters such as electrolyte and current density were also very significant for efficient pollutant removal. The results of this study suggest Magnéli phase electrodes as promising and cost-effective anode materials for industrial wastewater treatment, with Ti/Ti 4 O 7 NTA and Ti/Ti 4 O 7 being more efficient options.
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CARBON
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2020
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IF 8.821
Cai Xu,Leilei Jin,Xiaozhong Wang,Yingqi Chen,Liyan Dai
In heterogeneous catalysis , developing robust catalysts and preventing the metal leaching during the reactions still remain challenging. Herein, a porous honeycomb-like nanostructure with bimetallic Ce–Cr oxide supported on N-doped carbon was prepared via a facile in-situ pyrolysis method. The prepared catalyst was highly active, selective, and stable in the transformation of cyclohexane to KA oil with H 2 O 2 as the oxidant. The N-doped carbon served as an excellent support for the metal nanoparticles and greatly promoted their dispersion, and displayed a comparable or superior catalytic activity compared to the other traditional supports. It was found that the pyridinic N and pyrrolic N species of N-doped carbon were the main active sites for the metal immobilization , and the strong electronic interaction between N-doped carbon and Ce–Cr oxide was formed. The results revealed that the increased low-valence metal species might be responsible for the improved catalytic activity, and EPR analysis indicated that the hydroxyl radicals played a crucial role during the oxidation process . Besides, the catalyst can be easily separated and still remained stable after recycling seven times, making it a promising candidate for the catalytic oxidation of cyclohexane to KA oil under mild conditions.
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APPLIED CATALYSIS A-GENERAL
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2018
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IF 4.521
Xiaoqiang Wang,Yue Liu,Qingji Ying,Weiyuan Yao,Zhongbiao Wu
In this paper, a series of Nb modified Cu-Ce-Ti mixed oxides (Nb y CCT) were synthesized using wetness impregnation method for the selective catalytic reduction of NO with ammonia (NH 3 -SCR). The activity tests indicated that Nb y CCT catalysts had shown superior SCR performances. Among which, Nb 0.05 CCT catalyst exhibited a NO conversion of more than 90% within a broad operation temperature window (180–360 °C) under the GHSV of 40,000 h −1 . After that, corresponding characterizations were performed to correlate the physical structures and surface properties to catalytic performances. These results revealed that the strong interactions among the active phases induced by Nb addition could not only enhance the redox property of the catalysts but also inhibit the over-oxidation of NH 3 , which would be beneficial to SCR performance within a wide temperature range and good reaction selectivity. Furthermore, DRIFTS results suggested that the doping of Nb could promote the formation of NO 2 , thereby enhancing the “fast” SCR reaction process (Langmuir-Hinshelwood reaction pathway). Moreover, the Nb 0.05 CCT catalyst showed a better sulfur tolerance compared to Nb free catalyst that over 85% NO conversion could be retained after 12 h SCR reaction in the presence of SO 2 and H 2 O.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2016
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IF 3.205
Yushan Hou,Jianfang Wu,Elena Yu. Konysheva
Quantitative analysis of Cr-adsorption from a gas phase on CeO 2 , pure and doped BaCeO 3 was performed in combination with surface techniques and electrochemical impedance spectroscopy . The Cr-adsorption on BaCeO 3 is 3 times higher than on CeO 2 and it increases by 12–25% on In doping in Ba(Ce 1−x In x )O 3 (x = 0.1–0.3) in the temperature range of 600–700 °C. These perovskites adsorb chromium with the formation of a multi-phase surface layer containing BaCr 6+ O 4 and cerium oxide. Coexistence of small fractions of Cr 3+ and Cr 5+ cations in the surface layer was identified by X-ray photoelectron spectroscopy. The thickness of the surface layer and its morphology vary with temperature, affecting the conductivity of Ce containing perovskites below 700 °C. BaCrO 4 exhibits under air noticeably larger anisotropic thermal expansion than BaCeO 3 . The results indicate that high tolerance to Cr-gaseous species should be considered as an important criterion for further development of materials for proton-conducting SOFCs.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2024
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IF 4.9
Lian Yang,Haoran Qiu,Guoliang Liu,Jiang Chang,Shaoxia Yang,Feng Xiao
In this study, a series of novel thermo-responsive materials were synthesized using polyvinylidene fluoride, N-isopropylacrylamide (NIPAM) and graphene oxide (GO) via Ce (IV)-induced redox radical polymerization name as PNG. Thermo-responsive membranes were prepared by non-solvent induced phase separation. The results demonstrated that the C O and N-H stretching absorption intensities increased with the addition of NIPAM. XPS analysis demonstrated that the PNG1 membrane exhibited abundant functional group structure under the dosage of NIPAM at 1 g. The finger-like porous structure of membrane became longer and wider with the addition of NIPAM at 1 g, leading to a maximum porosity of 45.5 %. The CA decreased from 62.4 ° to 49.0 ° at 35 °C under the adding dosage of NIPAM at 1 g. The temperature-sensitive of PNG1 membrane was 35 °C. In addition, The PNG1 membrane had the lower R ir and higher flux recover than the others under the BSA rejection. According to the XDLVO theory analysis, the total interaction energy for PNG1 membrane achieved the maximum absolute values of −33.850 mJ/m 2 and −19.956 mJ/m 2 than the others under the temperature at 25 °C and 35 °C. This interaction influenced the adsorption between the pollutant and membrane surface, resulting in reversible fouling.
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