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ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY · 2022 · IF 7.129

Efficient Microcystis aeruginosa coagulation and removal by palladium clusters doped g-C3N4 with no light irradiation

Shihuan Lu,Xizi Li,Bingzhi Yu,Jiafeng Ding,Yuchi Zhong,Hangjun Zhang

Efficient treatment of cyanobacterial blooms in eutrophication waters by safe and reliable nanomaterials is a big challenge for reducing environmental health risks. Herein, a novel strategy combining palladium clusters (Pd n ) with g-C 3 N 4 nanocomposite was presented to achieve high-efficient removal of Microcystis aeruginosa cells through coagulation and breakage. Interestingly, 95.17% of algal cells (initial concentration of 5.6 × 10 6 cells mL −1 ) were promptly removed in the Pd/g-C 3 N 4 (5%) system within only 10 min and without visible light irradiation and persulfate activation. Both the release of potassium ion and microcystin during the removal process and the transmission electron microscope observations of Microcystis aeruginosa cells proved that the integrity of the algal cell membrane was destroyed. The removal of Microcystin-LR (MC-LR) were further confirmed in the next process. Pd metal interaction and breakage against algal cells may cause disruption of algal cells. This study describes a novel technology for the superfast removal of harmful algae and may provide a new insight into the control of cyanobacterial blooms in practical applications.

研究领域: 环境科学 · 微生物学
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SENSORS AND ACTUATORS B-CHEMICAL · 2022 · IF 9.221

An ESIPT fluorescent probe based on Staudinger reaction for detection of triphenylphosphine and tetrakis(triphenyl-phosphine)palladium

Yuhuan Zhang,Hongjuan Li,Shiguo Sun,Yongqian Xu

Triphenylphosphine (PPh 3 ) and tetrakis(triphenylphosphine)palladium (Pd(PPh 3 ) 4 ) are harmful at extremely low concentration, thus it is essential to explore selective and sensitive method to detect them. Based on Staudinger reaction mechanism, here we present a simple excited-state intramolecular proton transfer (ESIPT) fluorescent probe (HBTN) for detection of PPh 3 and Pd(PPh 3 ) 4 over other phosphine derivatives with differential channel fluorescence (enol and keto emission). The reaction-typed fluorescence probe with novel Staudinger reaction mechanism offers very low autofluorescence and a large signal-to-noise response signal, which is beneficial for the sensitive detection of PPh 3 and Pd(PPh 3 ) 4 . Moreover, HBTN can be used for efficiently detecting Pd(PPh 3 ) 4 residues in highly purified products and imaging PPh 3 in living cells.

研究领域: 分析化学 · 生物医学
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CATALYSIS TODAY · 2019 · IF 4.888

Enhanced catalytic performance of methane combustion over zeolite-supported Pd catalysts with the lanthanum

Yiquan Xie,Ling Zhang,Yiwen Jiang,Shichao Han,Liang Wang,Xiangju Meng,Feng-Shou Xiao

Catalytic combustion of CH 4 to CO 2 and H 2 O was studied over zeolite-supported Pd catalysts, and it was found that zeolite-supported Pd catalysts can present pronounced discrepancy in the catalytic performance of methane oxidation when Na-ZSM-5 was ion-exchanged with various cations of La, Ni, and Mg. Very interestingly, the Pd catalyst supported by NaLa-ZSM-5 exhibited the best result. Over an optimized catalyst, a complete conversion of methane can be achieved at around 320 °C, which is about 60 °C lower than the temperature needed for Pd/Na-ZSM-5. Physicochemical characterizations such as XRD, SEM, HRTEM, XPS, and ICP-OES techniques were used to investigate the factors influencing the catalytic activity and find out the reasons behind the discrepancy in the catalytic performance of methane combustion over these zeolite-supported Pd catalysts. Based on the characterization results, it is proposed that the Pd dispersion and its chemical states are major factors that govern catalytic performance of methane combustion over these catalysts. To the best of our knowledge, the optimal catalyst in this study stands out compared with other reported similar Pd catalysts for the catalytic combustion of methane in terms of activity.

研究领域: 化学工程 · 催化科学
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Journal of Materials Chemistry A · 2014 ·Vol. 3 ·期 6 ·2609-2616 · IF 0

Combining palladium complex and organic amine on graphene oxide for promoted Tsuji–Trost allylation

Qingshan Zhao,Yuanzhi Zhu,Zhen Sun,Yang Li,Guoliang Zhang,Fengbao Zhang,Xiaobin Fan

In this study, we develop a facile strategy to combine an organic amine with a palladium complex on graphene oxide (GO) as a cooperative catalyst for Tsuji–Trost allylation. A tertiary amine and palladium–diamine complex are simultaneously immobilized on a GO support through silylation and further in situ coordination processes. PdCl2 is employed as the palladium precursor, with no necessity for extra coordination ligands. Various characterizations confirm the successful preparation of the cooperative supported catalyst (GO–NEt2–2N–Pd). Systematic investigation reveals the immobilized palladium–diamine complex (GO–2N–Pd) with very low Pd loading is effective for Tsuji–Trost allylation, and incorporation of the tertiary amine shows a significant promoting effect towards the catalytic activity. GO–NEt2–2N–Pd can be readily recovered and recycled several times without reduction of its efficiency. Its excellent performance should be ascribed to synergistic catalysis effect, excellent support properties, and robust immobilization interaction.

研究领域: 催化化学 · 材料科学
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APPLIED CATALYSIS A-GENERAL · 2021 · IF 5.706

In situ hydrogenation of phenol to cyclohexanone on Pd/C with phosphotungstic acid at open atmospheric condition

Hui Chen,Jie He,Jinsheng Sun

The production of cyclohexanone, of industrial importance, is at a distance to environment friendly and efficiency. As a solution, a mild sustainable catalytic hydrogenation is presented herein, of phenol into cyclohexanone on Pd/C with potassium formate the hydrogen donor under open atmosphere. Some important reaction conditions, such as temperature, reaction time, catalyst, amount of potassium formate, etc. were investigated and analyzed. The positive growth was found to accelerate the conversion rate of phenol while reducing cyclohexanone selectivity by weakening the protection of phosphotungstic acid. Phosphotungstic acid was confirmed to be the co-catalyst exhibiting the highest activity under given conditions. Based on experiments, we have made reasonable assumptions about the reaction mechanism, while the reaction kinetics proves high reaction rates within a wide temperature range, indicating the reaction to be quick process. Furthermore, the good reusability and recyclability of Pd/C catalyst is verified to benefit future industrial applications.

研究领域: 化学工程 · 催化化学
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JOURNAL OF MATERIALS SCIENCE · 2021 ·Vol. 56 ·期 12 ·7308-7320 · IF 4.22

Direct oxidative esterification of alcohols catalyzed by a nitrogen-doped carbon black-supported PdBi bimetallic catalyst under ambient conditions

Hu Yongke,Xia Jiawei,Li Jin,Li Huaju,Li Yanxing,Li Shaozhong,Duanmu Chuansong,Li Bindong,Wang Xin

A highly efficient nitrogen-doped carbon black (NCB)-supported PdBi alloy nanocatalyst has been fabricated via a facile coreduction wet chemical approach. The optimal PdBi/NCB shows outstanding catalytic performance with broad substrate scope, good functional group tolerance towards direct oxidative esterification of alcohols under mild conditions in a heterogeneous catalytic system with air as the sole oxidant. A variety of benzylic and allylic alcohols were smoothly reacted with methanol and even with long-chain aliphatic alcohols, providing desired esters in good to excellent yields. Moreover, the as-prepared catalyst is easily recycled and can be reused at least five times without a significant loss of catalytic activity. Superior catalytic activity is mainly attributable to the unique structure of the catalyst, including synergetic electronic effect between Pd and Bi, as well as modulated surface character by acidification and N doping for better active components’ anchoring and dispersion, as well as reactants’ adsorption. This study provides a facial, practical, eco-friendly and efficient catalytic system for oxidative esterification of alcohols and shows promising prospect in industrial production.

研究领域: 化学 · 材料科学 · 催化
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY · 2020 · IF 3.306

A new palladium complex as a dual fluorometric and colorimetric probe for rapid determination of sulfide anion

Muhammad Amir Masood,Yuncong Chen,Shankun Yao,Shumeng Li,Weijiang He,Zijian Guo

A new BODIPY based Pd (II) complex, Pd-BDPA has been developed as a dual fluorometric and colorimetric probe for the detection of sulfide anion. The sensing ability is based on the interaction affinity of the Pd (II) towards the sulfide anion which is highly selective and immediate with a detection limit of 240 nM. The interaction between Pd (II) and sulfide is not only highly selective over the other common anions but also not interfered by their coexisting. This selective interaction between them leads to the regeneration of free ligand resulting in the dramatic changes in both fluorescence and absorption spectra. The fluorescent changes lead to quenching the emission spectra which is linear with the concentration of sulfide in the range of 1-10 μM. In addition to fluorescence quenching, the interaction also resulted in the significant color switching from purple to blue which was easily distinguished by the naked eye. Another important advantage is that the Pd-BDPA coated paper-based strips show the sulfide selectivity and sensitivity by the color changes as is in the solution form, revealing its practical utility more conveniently. In addition, the Pd-BDPA probe can also successfully be utilized for the determination of sulfide in real water samples with satisfactory recovery results indicating its feasibility for environmental samples.

研究领域: 分析化学 · 环境科学 · 生物化学
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Small · 2021 ·Vol. 17 ·期 52 ·2105643 · IF 13.281

The Dehydrogenation of H-S Bond into Sulfur Species on Supported Pd Single Atoms Allows Highly Selective and Sensitive Hydrogen Sulfide Detection

Bo Liu,Linjuan Zhang,Yuanyuan Luo,Lei Gao,Guotao Duan

The supported metal catalysts on scaffolds usually reveal multiple active sites, resulting in the occurrence of side reaction and being detrimental to the achievement of highly consistent catalysis. Single atom catalysts (SACs), possessed with highly consistent single active sites, have great potentials for overcoming such issues. Herein, the authors used SACs to modulate kinetic process of gas sensitive reaction. The supported Pd SACs, established by a metal organic frameworks-templated approach, promoted greatly the detection capacity to hydrogen sulfide (H 2 S) gas with a very high sensitivity and selectivity. Density functional theory calculations show that the supported Pd SACs not only increased the number of electrons transferring from H 2 S molecules to Pd SACs, but strengthened surface affinity to H 2 S. Moreover, the H  S bonds of H 2 S molecules absorbed on Pd atomic sites are more likely to be dehydrogenated directly into sulfur species. Significantly, quasi in situ XPS analysis confirmed the presence of sulfur species during H 2 S detection process, which may be a major cause for such detection signal. Based on these results, a suitable sensing principle for H 2 S gas driven by Pd SACs was put forward. This work will enrich catalytic electronics in chemiresistive gas sensing.

研究领域: 材料科学 · 催化化学 · 气体传感
✓ 已验证 DOI PubMed 高影响因子
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Particuology · 2024 · IF 4.1

Room-temperature hydrogen adsorption in Pd nanoparticle decorated UiO-66-NH2 via spillover

Jingchuan Wang,Junhong Luo,Yong Yao,Jiangfeng Song,Yan Shi

To improve room-temperature hydrogen storage, palladium (Pd) nanoparticles were innovatively decorated by carbon bridge onto the amino-group functioned Zr-terephthalate metal-organic framework (MOF) UiO-66 to reduce the diffusion energy barrier and then improve the hydrogen spillover effect. Powder X-ray diffraction shows broad Pd peak and retained UiO-66-NH 2 integrity after Pd decoration. The hydrogen uptake capacity show that UiO-66-NH 2 -Pd exhibits best hydrogen storage performance than UiO-66-NH 2 and pristine UiO-66. The hydrogen up taken in Pd decorated UiO-66 (UiO-66-NH 2 -1Pd) was close to 4 wt% under 20 MPa at room temperature. Density functional theory (DFT) calculations show that hydrogen adsorption energy of UiO-66-NH 2 -Pd was −0.5897 eV, which was much lower than that of UiO-66-NH 2 (−0.3716 eV) and UiO-66 (−0.2975 eV). Ultimately, Pd decorated NH 2 group functioned UiO-66 enable improve storage capacities through hydrogen spillover under ambient conditions which could satisfy the demand for sustainable energy, especially for the long-term storage energy media.

研究领域: 材料科学 · 能源科学
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CHEMISTRY-A EUROPEAN JOURNAL · 2024 · IF 3.9

Hollow UiO-66-NH2 encapsulated Pd catalysts for highly selective hydrogenation of furfural to furfuryl alcohol

Bo Zhao,Yao Yao,Kexin Huang,Jiaxin Li,Minjie Chen,Chao Liu,Hongjian Xu,Xinyu Zhao,Ganggang Chang

The selective hydrogenation of furfural (FFA) to furfuryl alcohol (FA) is regarded as attractive transformation to achieve the sustainable synthesis of value-added chemicals from biomass resources. However, the conventional supported catalysts are significantly restricted by their narrow pore size, ununiform dispersion and easy leaching or aggregation of catalytic sites. Herein, we designed hollow UiO-66-NH2 as the support to encapsulate Pd nanoparticles (Pd@H-UiO-66-NH2) to achieve the highly active and selective conversion of FFA to FA. Benefiting from the void-confinement effect and substrate enrichment of hollow structure, as well as the surface wrinkles, the as-prepared catalyst Pd@H-UiO-66-NH2 exhibited 96.8 % conversion of FFA with satisfactory selectivity reaching up to 92.4 % at 80 °C, 0.5 MPa H2 in isopropanol solvent within 6 h. More importantly, as-prepared Pd@H-UiO-66-NH2 catalyst exhibited excellent long-term stability, as well as good universality toward a series of hydrogenation of unsaturated hydrocarbons.

研究领域: 化学工程 · 催化材料科学
✓ 已验证 产品关联 DOI PubMed 高影响因子
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Reaction Kinetics Mechanisms and Catalysis · 2024 ·Vol. 137 ·期 3 ·1701-1720 · IF 1.7

Triggering effect of ultra small Pd nanoparticles on hydrogenation of tetraacetyldibenzylhexaazaisowurtzitane (TADBIW)

Guo Kailiang,Liu Shuang,Men Yong,Li Lin,Hu Jiajia,Xu Junzhe,Sun Chenghui,Wei Gaixia,Wang Jinguo,He Shan,Wu Bin,Huang Xiaohui

Herein, we prepared Pd nanoparticle (NP) catalysts using XC-72 carbon supports through a tailored deposition–precipitation method. Our primary objective was to unravel the size effects of Pd NPs on hydrogenation of tetraacetyldibenzylhexaazaisowurtzitane (TADBIW), a pivotal intermediate for synthesis of high energy density materials hexanitrohexaazaisowurtzitane (CL-20). The controlled modulation of Pd NP size ranged from a mere 1.8 nm to 7.4 nm. Remarkably, our investigations into TADBIW hydrogenation unveiled a fascinating trend: the ultrasmall-sized Pd NPs with a diameter of 1.8 nm exhibited excellent yield and reaction rates. In stark contrast, their larger-sized counterparts demonstrated diminished catalytic activities. To disclose the size-dependent nature, various characterization techniques were employed, including XRD, TEM, XPS, CO and H 2 pulse chemisorption. The comprehensive analysis revealed that the ultrasmall-sized Pd possessed more positively charged sites and exhibited higher dispersion. This unique configuration facilitated an accelerated adsorption of hydrogen and the electron-rich substrate TADBIW. Notably, this phenomenon led to a reduction in the activation energy through a thermodynamic effect, thereby enhancing overall catalytic performance. Our results strongly suggested that the ultrasmall-sized Pd NPs can exert a dominated influence on the physical and chemical states of the active sites, playing a key role in triggering the adsorption and activation of the substrate TADBIW. These findings not only deepen our understanding of the intricate connections between Pd NP size and catalytic activity but also open new avenues for advancing the design and optimization of catalysts in the hydrodebenzylation methodologies and synthesis of related compounds.

CAS / MDL: 75-05-8 64-19-7 68-04-2
研究领域: 材料科学 · 催化化学 · 能源材料
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ChemCatChem · 2025 · IF 3.9

Structure Evolution of Pd/C Catalyst in the Catalytic Dehydrogenation of Dodecahydro-N-ethylcarbazole: Effects of Pd Species and Particle Size

Jingrong Li,Tingting Xiao,Xinluona Su,Qihang Gong,Peikai Luo,Jian Li,Haiyang Cheng,Fengyu Zhao

Graphical The evolution of the geometric structure and electronic states of Pd species was revealed for Pd/C catalysts in catalyzing the dehydrogenation of 12H-NECZ. The oxidized Pd δ+ species was reduced to Pd 0 species with finely-dispersed on the surface of support to generate H 2 with a high efficiency of 98.3%. The dehydrogenation of liquid organic hydrogen carriers is of significant potential for hydrogen energy applications. We successfully synthesized a highly efficient and stable Pd/C catalyst featuring ultrasmall (2.22 nm) and stable Pd nanoparticles via the deposition–precipitation method for the dehydrogenation of dodecahydro- N -ethylcarbazole. Interestingly, the Pd structure evolves during the reaction, with the Pd 2+ species on Pd/C catalyst re-dispersing into uniformly small-sized Pd 0 nanoparticle under reaction conditions. The conventional thermal treatment of calcination–reduction typically results in larger Pd particles due to the stronger metal-support interaction. Kinetic studies revealed the oxidation state of Pd 2+ species (Pd(OH) 2 , PdO) is more active for the dehydrogenation reaction compared to the metallic state Pd 0 species. The in situ structure evolution induced ultrasmall Pd nanoparticles (2.22 nm) with a constant Pd 0 /Pd 2+ ratio, achieving a high efficiency (98.3%) of H 2 release from 12H-NECZ dehydrogenation at 180 °C. This work provides a simple method for preparing highly dispersed Pd/C catalyst with stable ultrasmall Pd particles, offering valuable insights to researchers in the field of supported metal catalysts.

研究领域: 催化化学 · 材料科学 · 能源化学
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