WATER SCIENCE AND TECHNOLOGY
·
2016
·Vol. 74
·期 3
·639-646
·
IF 1.064
Zhang Zhen,Zhang Junya,Ye Xiaokun,Hu Yongyou,Chen Yuancai
Ethylenediaminetetraacetic acid (EDTA) forms stable complexes with toxic metals such as nickel due to its strong chelation. The electro-Fenton (EF) process using a cathode made from palladium (Pd), reduced graphene oxide (RGO) and carbon felt, fed with air, exhibited high activities and stability for the removal of 10 mg L −1 EDTA-Ni solution. Pd/RGO catalyst was prepared by one-pot synthesis; the scanning electron microscopy and X-ray diffraction analysis indicated nanoparticles and RGO were well distributed on carbon felt, forming three dimensional architecture with both large macropores and a mesoporous structure. The cyclic voltammetric results showed that the presence of RGO in Pd/RGO/carbon felt significantly increased the current response of two-electron reduction of O 2 (0.45 V). The key factors influencing the removal efficiency of EDTA-Ni, such as pH, current and Fe 2+ concentration, were investigated. Under the optimum conditions, the removal efficiency of EDTA-Ni reached 83.8% after 100 min EF treatment. Mechanism analysis indicated that the introduction of RGO in Pd/RGO/carbon felt significantly enhanced the electrocatalytic activities by inducing •OH in the EF process; direct H 2 O 2 oxidation still accounted for a large amount of EDTA-Ni removal efficiency.
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高影响因子
FUEL
·
2021
·
IF 6.609
Dawang Chu,Zhicheng Luo,Yingying Xin,Chengzhen Jiang,Shaofeng Gao,Zhihao Wang,Chen Zhao
The chemo-catalytic production of ethanol from nonedible lignocellulosic biomass is essential for mitigating energy shortage. In this work, we developed a multifunctional Pd-Cu-WO x /SiO 2 catalyst for the one-pot aqueous-phase conversion of cornstalk-derived cellulose to ethanol with a yield of 42.5C% at 300 °C and 4 MPa H 2 . Kinetic studies demonstrated that the transformation of cellulose to ethanol followed a number of consecutive steps namely, cellulose hydrolysis to glucose with H + in hot water (k 1 ), glucose conversion to glycolaldehyde over W species (k 2 ), glycolaldehyde hydrogenation to ethylene glycerol (EG) over Pd (k 3 ), and EG hydrogenolysis to ethanol over Cu (k 4 , rate-determining step). The individual rates were well balanced on Pd, Cu, and WO x species to achieve an ethanol formation rate of 0.163 g·g Cat . −1 h −1 . The addition of Au to Cu-WO x species led to a relatively low k 3 and thus the formation of a substantial amount of humins, while the Ru introduction catalyzed the over-hydrogenolysis of ethanol to methane and ethane with a high rate, thereby lowering the selectivity to ethanol. The characterization results showed that both the electronic properties of Cu + species and the Cu + /Cu 0 ratio on the Pd-Cu-WO x /SiO 2 catalyst contributed to a specific C O bond cleavage, especially for EG hydrogenolysis to ethanol during the cellulose conversion.
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AICHE JOURNAL
·
2023
·Vol. 69
·期 6
·e18049
·
IF 3.7
Fengyu Zhang,Chenglin Miao,Qian Wang,Mingyu Gao,Dianqing Li,Junting Feng
Aiming at controllable modulating metal−support interactions to achieve an optimal trade-off of geometric/electronic effect in supported catalysts, we developed a reliable approach based on the typical 2D material layered double hydroxide (LDHs). A series of TiO x /Pd/MgTiAl-MMO-X catalysts with adjustable interfacial effect were acquired by loading PdCl 4 2− precursor and further preciously adjusting the topological reduction temperature, based on the regulatory effect of Mg–O–Ti–O–Al–O structure in the support on the reducibility and mobility of Ti 4+ . The catalysts with semi-continuous and accessible TiO x /Pd interface, confirmed by AC-HAADF-STEM, CO chemisorption, XPS, exhibit much higher H 2 O 2 yield than the catalyst with over-encapsulation structure. The TiO x /Pd/MgTiAl-MMO-450 catalysts possessed optimal geometric and electronic structure exhibited the highest activity with TOF of 9.75 s −1 , excellent H 2 O 2 yield of 11.4 g/L, as well as good stability.
研究领域:
催化化学
·
材料科学
·
化学工程
·
纳米材料
·
绿色化学
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高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2026
·
IF 14.3
Tao Li,Wan Wang,Jiawei Chen,Yue Wang,Xiangbin Cai,Lini Yang,Xin Liu,Jiangyong Diao,Zarrin Es'haghi,Lixin Xia,Li Jin,Guoqing Wang,Hongyang Liu
The development of highly efficient nanozymes faces challenges of insufficient catalytic activity and low atom utilization. Atomically dispersed metal nanozymes have received widespread attention due to their high atomic utilization efficiency and exceptional catalytic activity. Bimetallic catalysts demonstrated enhanced catalytic performance owing to synergistic geometric and electronic effects arising from heterometallic interactions. Herein, we report an atomically dispersed palladium-iron bimetallic cluster nanozyme, in which fully exposed Pd clusters bonded to adjacent Fe atomic clusters are anchored onto defect-rich nanodiamond-graphene supports (PdFe/ND@G). The Pd-Fe interfacial sites fabricated in atomically dispersed bimetallic clusters deliver abundant oxygen activation sites for high-efficiency catalytic reactions and exhibit enhanced oxidase-like catalytic activity, demonstrating superior enzymatic activity and antibacterial performance compared to monometallic Pd and Fe clusters, while surpassing those of previously reported nanozymes. DFT calculations reveal that, compared to monometallic Pd clusters, atomically dispersed Pd-Fe clusters synergistically catalyze O 2 cleavage into OO* intermediates via Pd-Fe interfacial sites while exhibiting lower energy barriers, which is the critical factor for their enhanced enzyme-like activity. This study provides novel insights into constructing highly efficient atomically dispersed bimetallic cluster nanozymes.
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产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2018
·
IF 4.439
Zhanglong Guo,Yuefeng Liu,Yan Liu,Wei Chu
In this study, SiC supported Pd nanoparticles were found to be an efficient catalyst in acetylene selective hydrogenation reaction. The ethylene selectivity can be about 20% higher than that on Pd/TiO 2 catalyst at the same acetylene conversion at 90%. Moreover, Pd/SiC catalyst showed a stable catalytic life at 65 °C with 80% ethylene selectivity. With the detailed characterization using temperature-programmed reduction (H 2 -TPR), powder X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), N 2 adsorption/desorption analysis, CO-chemisorption and thermo-gravimetric analysis (TGA), it was found that SiC owns a lower surface area (22.9 m 2 /g) and a broad distribution of meso-/macro-porosity (from 5 to 65 nm), which enhanced the mass transfer during the chemical process at high reaction rate and decreased the residence time of ethylene on catalyst surface. Importantly, SiC support has the high thermal conductivity, which favored the rapid temperature homogenization through the catalyst bed and inhabited the over-hydrogenation of acetylene. The surface electronic density of Pd on Pd/SiC catalyst was higher than that on Pd/TiO 2 , which could promote desorption of ethylene from surface of the catalyst. TGA results confirmed a much less coke deposition on Pd/SiC catalyst.
研究领域:
催化化学
·
材料科学
·
化学工程
·
纳米技术
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2020
·
IF 3.573
Yanyan Wang,Yu Liu,Jiyang Li,Yuanyuan Liu,Weiqiang Zhang,Mingming Yang,Yajun Jian,Ping Zuo,Ziwei Gao
The position of Pd species in/on zeolites is crucial for the activity of metal/metal oxide catalysts. It is still a challenge to highly disperse and stabilize the metal species on zeolites and shorten diffusion paths to maintain high catalytic activity. Here, we report an effective strategy for preparing highly efficient zeolite-supported Pd(II) catalysts by positioning Pd(II) species on the surface of a zeolite with an anion framework based on the principle of charge balance. The catalyst was prepared in situ in a C–C cross-coupling reaction. Due to the change in the metal–support interaction, Pd species have migrated from the inside to the surface of the zeolite, which shortens the diffusion path of reactants and thus ensures the high activity of the catalyst. Pd species exhibit aggregation resistance in alkaline systems and tend to be confined in the traps with high charge density. Compared to unactivated Pd@USY, the efficiency of the activated catalysts has at least doubled in catalyzing the Sonogashira and Suzuki–Miyaura reactions. This study represents a new activation approach for zeolite-supported Pd catalysts, which may help to design efficient catalysts.
研究领域:
催化化学
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材料化学
·
有机合成
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纳米催化
·
多相催化
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2026
·
IF 9.6
Li-Yong Liu,Yun-Qi Dou,Maarten Bransen,Alfons van Blaaderen,Tian-Song Deng,Xiaoyu Zhao,Dechao Yu
Combining noble metal nanoparticles with electron acceptors, such as semiconductors or non-plasmonic metals, significantly enhances photocatalytic performance. However, optimizing multi-material combinations for superior catalytic efficiency remains challenging. In this study, we present a method for synthesizing composite structures by reducing Cu 2+ ions with hydrazine hydrate, forming gold nanorods (AuNRs) decorated with dendritic Cu 2 O shells. The influence of CTAB on Cu 2 O deposition sites was investigated, and ternary composite nanoparticles were further synthesized by incorporating Pd or Pt into the AuNR-Cu 2 O system (AuNR@Pd(Pt)-Cu 2 O). The photocatalytic performance of these nanostructures was evaluated by catalyzing methyl orange (MO) under light irradiation. Results showed that AuNR@Pt-Cu 2 O nanoparticles exhibited catalytic performance 35.7 times higher than that of pure Cu 2 O nanoparticles. This enhancement is attributed to efficient charge transfer and photothermal effects facilitated by the ternary structure. These findings provide valuable insights into plasmonic heterostructure design and open new avenues for developing high-performance photocatalysts for energy and environmental applications.
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PubMed
高影响因子
ACTA PHYSICO-CHIMICA SINICA
·
2026
·
IF 13.5
Xincan Zhou,Xueyao Wang,Xiaokang Chen,Di Lan,Yuting Gao,Xiaoxia Wang,Daohao Li,Shuchao Zhang,Lijie Zhang,Guanglei Wu
Pd-based materials as the promising catalysts for ethanol oxidation reaction (EOR) are still intrinsically limited by the surface electronic-structure trade-off between ethanol adsorption and CH 3 CO intermediate desorption. Herein, the Pd supported on N/S co-doped carbon (Pd@SNC) catalyst is synthesized, in which the doped S and N atoms could transfer moderate amounts electron to Pd, leading to opportune electron structure of Pd. Moreover, the moderate negative shift of d -band center demonstrate that the opportune Pd electron structure can strengthen adsorption of ethanol/OH − and promote the desorption of intermediate (CH 3 CO*), which may facilitate the kinetics. As a result, Pd@SNC exhibiting the highest catalytic activity for EOR (945.49 mA mg Pd −1 ), surpassing to that of Pd@NC and Pd@C. Due to the fact that the electronic structure of Pd is properly regulated by co-doped N and S atoms, as shown by the theoretical calculation results, Pd@SNC exhibits the lowest reaction energy barrier of the dehydrogenation during the process of EOR.
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产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2025
·Vol. 36
·期 13
·e17378
·
IF 19
Zhenxu Li,Tongtong Qi,Xinhua Zhao,Yi Zhang,Zhu Zhang,Tingting Wang,Xuze Xiao,Dachi Yang
Reliable methane (CH 4 ) sensing is highly desired in the underground pipe networks, and even low-concentration CH 4 leakage may cause disasters. However, it often suffers from instability and sluggish response caused by harsh working conditions (e.g., high humidity). Here, cerium oxide hollow nanospheres decorated with palladium and palladium oxide nanodots (Pd-PdO NDs / CeO 2 HNSs) are reported for stable and fast CH 4 sensing, which have been prepared via combined bubble confinement and in situ photochemical deposition. As-prepared Pd-PdO NDs / CeO 2 HNSs are hollow nanospheres of ≈0.96 µm in diameter. Beneficially, the sensing materials exhibit 3 s fast response and 0.1 ppm limit of detection. Further, Pd-PdO NDs / CeO 2 HNSs show excellent sensing stability of 510 days stability, 74% relative humidity tolerance, and 100 cycling stability. Theoretically, such outstanding CH 4 sensing performance is attributed to interface-coupled modulation between Pd-PdO NDs and CeO 2 HNSs, in which Pd-PdO NDs serve as catalytic centers, while CeO 2 HNSs act as both oxygen vacancy modulator and structural optimizer. Compared with a commercial sensor, Pd-PdO NDs / CeO 2 HNSs present superior response / recovery time, and a sensor prototype has been built to simulate the detection of CH 4 leakage with reliable responses.
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高影响因子
APPLIED CATALYSIS A-GENERAL
·
2026
·
IF 4.8
Ying Gao,Jinxing Long
Conversion of ethyl levulinate to GVL was proposed using Pd 4 /UiO-66-NH 2 . • Pd 4 /UiO-66-NH 2 was constructed via a post-synthetic modification strategy. • Synergistic effects between Pd species and acidic sites drive superior performance. • GVL yield of 90% with 98.9% selectivity was achieved under 170 ℃ and 1.0 MPa H 2 . • The catalyst shows good recyclability, and can be reused for at least five runs. An efficient strategy is proposed for direct hydrogenation of ethyl levulinate (EL) to γ-valerolactone (GVL) using a highly dispersed palladium nanoparticles supported on the UiO-66-NH 2 framework (Pd/UiO-66-NH 2 ), which was prepared via a facile post-synthetic modification by anchoring palladium (Pd) nanoparticles on the framework's native -NH 2 groups. Under optimized conditions (170 °C, 1.0 MPa H 2 ), 90% yield and 98.9% selectivity of GVL were shown when the reaction was catalyzed by Pd 4 /UiO-66-NH 2 in cyclohexane. Catalyst characterization using XRD, N 2 adsorption-desorption, FT-IR, TEM, TGA, XPS and H 2 -TPR, confirmed that an intensive synergistic effect existed between the Pd and the acidic sites, which is responsible for the superior performance of Pd@UiO-66-NH 2 . The solvent effect and the feedstock adaptability were also investigated. Furthermore, the catalyst of Pd 4 /UiO-66-NH 2 demonstrated good stability and reusability, where no significant activity loss was shown even after five consecutive cycles. Therefore, this study provides new insights for efficient upgrading biochemical. Download: Download high-res image (188KB) Download: Download full-size image
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International Journal of Coal Science & Technology
·
2026
·Vol. 13
·期 1
·51
·
IF 10.1
Deng Wenyao,Bao Guirong,Li Kongzhai,Wang An,Ji Xuewu,Liu Li,Gao Peng,Wang Hua,Luo Jia
C = C and C = O selective hydrogenation in aromatic compounds is a key capability of supported active metal catalysts, leading to numerous practical applications. Here, carbon dots (CDs) material was produced by microwave-assisted hydrothermal method, and used as the carrier and reducing agent to develop PdAg/CDs composite catalyst. PdAg/CDs fabricated by photochemical reduction with UV-light demonstrated high selectivity for hydrogenation of cinnamic aldehyde (CAL) into hydrocinnamic alcohol (HCOL). With PdAg/CDs, 100% of CAL conversion and 90.0% of selectivity to HCOL were obtained at 140 °C, 3 h and 1 MPa H 2 in water. The improved catalytic performance of the PdAg/CDs catalyst was mainly due to the formation of Pd-Ag alloy and synergetic effect between Pd and Ag.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Chunmin Guo,Ke Li,Ruoxi Liu,Yiwei Peng,Yang Sun,Xiaoliang Wang,Hongyu Sun,Shetian Liu,Yanlong Yu
Photo-Electrochemical Synergistic Strategy for Constructing Oxygen-Vacancy-Rich Pd/CeO2/NF. • Ultralow Pd loading delivers an exceptional mass activity of 362.57 min-1 gPd-1，complete 4-CP removal in 120 min, and outstanding durability (>95%, 10 cycles). • SMSI induces an oxygen-vacancy-rich CeO2 surface that promotes water activation to generate abundant H* species. • DFT calculations rationalize the enhanced performance: interfacial charge transfer (~0.52 e) from Pd to CeO2 optimizes ΔGH* at the Pd/CeO2 interface, validating the spatially decoupled hydrogen spillover mechanism. Chlorinated organic compounds (COCs) pose severe threats to ecological systems and human health owing to their high toxicity and recalcitrance to degradation. Electrocatalytic hydrodechlorination (EHDC) has emerged as a promising remediation strategy, as it directly drives C Cl bond cleavage via cathodic electron transfer without requiring exogenous chemical reductants and operates under mild conditions. Palladium (Pd), with its unique d-electron configuration, exhibits a near-optimal hydrogen adsorption free energy and is therefore well-suited for this reaction. However, conventional Pd catalysts suffer from low atomic utilization efficiency and severe competing hydrogen evolution reaction (HER). To address these limitations, a photo-assisted electrodeposition strategy was developed to simultaneously achieve high dispersion of Pd active sites and precise regulation of interfacial electronic structure. Ultraviolet irradiation of the CeO 2 support generated photoelectrons that induced in-situ reduction and anchoring of Pd precursors at oxygen vacancy defect sites, effectively suppressing Pd migration and aggregation. Consequently, highly dispersed Pd nanoparticles (~4.65 nm) were obtained at an ultralow Pd loading of 0.1326 wt%, maximizing precious-metal atom utilization efficiency. Furthermore, strong metal–support interactions (SMSI) between Pd and CeO 2 induced directional interfacial electron transfer from Pd to CeO 2 (~0.52 e), creating an electron-rich Pd-CeO 2 interface. This electronic reconstruction precisely modulated the hydrogen adsorption free energy and effectively suppressed excessive H* accumulation on Pd, thereby mitigating the competing HER. This work provides a new interfacial engineering strategy for designing EHDC catalysts with low precious-metal loading and high atom utilization efficiency, while elucidating the mechanism by which oxygen vacancies regulate hydrogen spillover for enhanced catalytic performance. Download: Download high-res image (155KB) Download: Download full-size image
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