NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 18
·8739-8751
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IF 3.925
Quansheng Wu,Songhua Zhou,Chengbing Fu,Jiesong Zhang,Bo Chen,Hongyan Pan,Qian Lin
For the mono-metal Pd based catalysts, the O–O bond in O2 and H2O2 is easily dissociated due to the higher energy sites of Pd, which decreases the selectivity and productivity of H2O2. To address this issue, non-noble metals M (M = Sn, Fe, Co, Ni) were doped into palladium precursors to create a series of yolk–shell structure bimetallic catalysts Pd–M@HCS (H = hollow; C = carbon; S = sphere) with Pd–M as the core and porous carbon as the shell. The results indicated that the catalyst Pd–M@HCS doped with Sn, Fe, Co, and Ni has a weak dissociation ability for O2, and both the adsorption and dissociation ability for H2 are improved. Of these catalysts, the catalyst Pd–Sn@HCS gives the best performance, which is benefited by the suitable Pd–Sn nanoparticle size and the best Pd2+/Pd0 ratio. The influence of the nPd/nSn ratio in the Pd–Sn@HCS system on catalyst performance was further explored, and the findings revealed that Pd–Sn@HCS had the best catalytic activity and stability when the nPd/nSn ratio was 2. The catalyst's H2 conversion, H2O2 selectivity, and productivity were 35%, 97%, and 3961 mmol gPd−1 h−1, respectively. After 10 cycles, the H2O2 productivity of this catalyst remained at 92.1%, which was greater than the H2O2 productivity of the typical Pd-based catalyst Pd/C, which stayed at 37% under the same conditions.
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ACS Nano
·
2021
·
IF 15.881
Shaoda Huang,Shuanglong Lu,Shun Gong,Qiuju Zhang,Fang Duan,Han Zhu,Hongwei Gu,Weifu Dong,Mingliang Du
Engineering the morphology and electronic properties simultaneously of emerging metallene materials is an effective strategy for enhancing their performance as oxygen reduction reaction (ORR) electrocatalysts. Herein, a highly efficient and stable ORR electrocatalyst, Fe-doped ultrathin porous Pd metallene (Fe–Pd UPM) composed of a few layers of 2D atomic metallene layers, was synthesized using a simple one pot wet-chemical method and characterized. Fe–Pd UPM was measured to have enhanced ORR activity compared to undoped Pd metallene. Fe–Pd UPM exhibits a mass activity of 0.736 A mgPd–1 with a loss of mass activity of only 5.1% after 10 000 cycles at 0.9 V versus the reversible hydrogen electrode (vs RHE) in 0.1 M KOH solution. Density functional theory (DFT) calculations reveal that the stable Fe dopant in the inner atomic layers of Fe–Pd UPM delivers a much smaller overpotential during O* hydrogenation into OH*. The morphology, porous structure, and Fe doping were verified to have enhanced ORR activity. We believe that the rational design of metallene materials with porous structures and interlayer doping is promising for the development of efficient and stable electrocatalysts.
研究领域:
材料科学
·
电化学
·
理论计算
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JOURNAL OF ORGANIC CHEMISTRY
·
2023
·
IF 3.6
Chenxu Zheng,Zhi-Jiang Jiang,Ke Jin,Qian Wang,Jian-Fei Bai,Gang Xu,Zhanghua Gao
As a representative scaffold of alkaloids, indoles have been extensively subjected to deuteration, but the regioselective C4 labeling has not been achieved due to its low reactivity. In this work, a Pd-catalyzed deuterium labeling at the indole’s C4 position has been developed under the strategy of transient directing, using D2O as a deuterium source. The substituent effect is found to be crucial in facilitating this H/D exchange process, where the reversing C–D bond formation favors an electron-enriched ligation contrary to its C–H halogenation counterpart.
研究领域:
有机化学
·
药物化学
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Nano Research
·
2021
·Vol. 14
·期 7
·2441-2450
·
IF 8.897
Peng Lingxin,Tian Han,Cui Xiangzhi,Su Liang,Meng Ge,Ma Zhonghua,Cao Shaowen,Shi Jianlin
Developing anode catalysts of substantially enhanced activity for hydrogen oxidation reaction (HOR) and anti-CO poisoning performance is of great importance for the application of proton exchange membrane fuel cells (PEMFCs). Herein, we report Pd cluster in situ decorated urchin-like W 18 O 49 (WO 2.72 ) electrocatalysts by a photo-reduction method for high performance HOR. The synthesized Pd-WO 2.72 -L composite of low loading amount of 0.44 wt.% Pd by Xenon light reduction exhibits markedly high HOR catalytic activity and stability in 0.5 M H 2 SO 4 , and the specific HOR current density and mass activity of Pd-WO 2.72 -L are ∼ 1.5 and ∼ 80 times those of 20 wt.% Pt/C catalyst, respectively. Moreover, excellent anti-CO poisoning ability has also been obtained. The excellent HOR activity and anti-CO poisoning performance of Pd-WO 2.72 -L have been discussed mainly in terms of the dual synergetic catalytic effects between Pd and WO 2.72 : Pd activation to Pd δ+ by the electron transfer from Pd to W promotes the hydrogen adsorption and activation to H* species, which results in largely elevated HOR activity; Pd degradation due to the CO poisoning is effectively prevented by WO 2.72 , which is responsible for the excellent CO-tolerance performance.
研究领域:
材料科学
·
电化学
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JOURNAL OF CONTROLLED RELEASE
·
2020
·
IF 7.727
Mengshi Jiang,Wei Li,Chunqi Zhu,Xiang Li,Junlei Zhang,Zhenyu Luo,Bing Qin,Yongzhong Du,Lihua Luo,Jian You
The application of nanocarriers as drug delivery system for chemotherapeutic drugs has become a research hotspot in cancer treatment. Chemotherapy with high tumor-targeting accuracy and drug release specificity is the key to improve the efficacy of tumor chemotherapy and reduce the side effects caused by repeated doses drugs. Here, we synthesized a redox-sensitive nano-micelle formed by hyaluronic acid (HA) conjugated with d -α-tocopherol succinate (TOS) using a disulfide bond as the linker (HA-SS-TOS, HSST), which could actively accumulate to the tumor sites and metastasis cancer cells with high expression of CD44. The micelles could dissociate under the high GSH level in cancer cells, triggering a release of paclitaxel (PTX). Surprisingly, the precise chemotherapy instead induced a suppressive tendency of immune system, manifested by a significant increase in TGF-β, which weakened the therapeutic effect of micelles. Moreover, the high levels of TGF-β might be related to the increased drug-resistance of cancer cells. Research has shown that PD-1 pathway blockade can result in reduction in TGF-β expression, thus, a PLGA microsphere encapsulating PD-1 antagonist peptides A12 ( [email protected] ) was further prepared to activate the host immune response. Our data indicated that PTX-loaded HSST could accurately “find” the tumors as well as metastasis cancer cells, and efficiently kill most of them. The joining of a durable PD-1 blockage significantly boosted the efficacy of [email protected] on multiple tumor models, including lung metastatic tumors and even multidrug-resistant tumors. Thus, our work presented an optimal chemo-immunotherapy combined system, which shows profound significance for future cancer therapy in clinic.
研究领域:
癌症治疗
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纳米技术
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药学
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免疫学
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Molecular Catalysis
·
2026
·
IF 4.3
Shukang Ti,Dongmei Yue
Pd/DUT-5 is an efficient catalyst for NBR hydrogenation to HNBR. • High hydrogenation activity was achieved under mild conditions. • Metal-support interactions stabilize electron-enriched Pd δ+ species. • Pd δ+ species enhance catalytic activity and chemoselectivity. • DFT reveals low-barrier heterolytic H 2 activation at Pd δ+ –μ 2 O - sites. Hydrogenated nitrile butadiene rubber (HNBR), produced via the selective hydrogenation of nitrile butadiene rubber (NBR), has attracted considerable interest because of its excellent overall performance. However, the development of efficient and selective catalytic systems for NBR hydrogenation under mild conditions remains challenging, particularly when both activity and cost-effectiveness are required. Herein, Pd nanoparticles were immobilized on the Al-based metal-organic framework DUT-5, and the influences of Pd precursor salts and pretreatment conditions on catalytic hydrogenation performance were systematically investigated. The results show that using Pd(OAc) 2 as the precursor in combination with relatively low reduction temperatures promotes the formation and stabilization of electron-enriched Pd δ+ species through metal-support interactions, leading to excellent low-temperature activity and good reusability, with the hydrogenation degree remaining 94.5% after three cycles. Density functional theory calculations using C 2 H 4 as a model substrate further reveal that Pd δ+ sites cooperatively interact with μ 2 O - moieties to facilitate H 2 activation and subsequent hydrogen transfer through a heterolytic cleavage pathway with reduced energy barriers. These results provide a mechanistic basis for the efficient hydrogenation of NBR under mild conditions. Overall, this work demonstrates an effective and economical strategy for HNBR production and offers new insights into the design of highly active and chemoselective catalysts for NBR hydrogenation. Download: Download high-res image (205KB) Download: Download full-size image
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Catalysts
·
2026
·Vol. 16
·期 2
·167
·
IF 4.5
Zhipeng Su,Xueyin Zhang,Tiehong Chen
Pd-based catalysts with different Pd species (Pd ions, Pd clusters, and Pd nanoparticles) in USY were synthesized for naphthalene hydrogenation reaction. Among the catalysts, Pd clusters were prepared by controlled aggregation of Pd ions during the hydrogenation reaction with the assistance of physically adsorbed water in zeolite micropore. The coordination state and electronic structure of Pd species on these catalysts were analyzed to reveal the structure–performance relationship. Due to the high dispersion and optimized electronic structure, Pd clusters showed the highest activity for naphthalene hydrogenation compared to Pd ions and Pd nanoparticles.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2026
·
IF 12.2
Weiting He,Xin Wang,Zishao Li,Daoyuan Zu,Kuanchang He,Kui Yang,Wei Li,Cheng Chao Li,Jinxing Ma
Electrochemical dehalogenation is a promising approach for removing persistent halogenated organic pollutants from water, but its practical application is often constrained by limited mass transfer and high energy demand in conventional batch reactors. Here, we report a self-separating flow cathode system using Pd-loaded Ti4O7 microparticles (Pd/Ti4O7), integrated with a porous Ti filter that enables in situ particle retention and recycling. With an optimized Pd loading of 0.5 wt %, the system achieved 93- and 13-fold faster diclofenac (DCF) dechlorination than systems without Pd/Ti4O7 and with Ti4O7 alone, respectively, while significantly reducing predicted biotoxicity. Efficient dehalogenation was further demonstrated for multiple chlorinated organic pollutants. Direct electron transfer (DET), rather than atomic hydrogen-mediated reduction, dominates the dehalogenation pathway, which confers strong resistance to common water matrix interferences. A single-pass system removed 99% of DCF from municipal wastewater within 7 min at an energy cost of 0.26 kWh·m–3, comparable to or lower than state-of-the-art technologies. Collectively, these results establish Pd/Ti4O7 self-separating flow cathodes as a robust and scalable platform for electrochemical dehalogenation, while highlighting remaining challenges related to material cost and life-cycle impacts.
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JOURNAL OF ORGANIC CHEMISTRY
·
2026
·
IF 3.3
Lu Wang,Yulu Du,Yanrong Zhu,Bing Zhang,Wenhui Wang,Ying Fu,Zhengyin Du
A palladium-catalyzed tandem Heck cyclization of N-(2-iodoaryl)acrylamides with N-methylanilines and ClCF2COONa has been developed for the synthesis of carbamoyl-substituted oxindoles bearing an all-carbon quaternary stereocenter, wherein difluorocarbene serves as the carbonyl source. This method operates under mild conditions, exhibits a broad substrate scope, and features operationally simple and safe procedures. Moreover, it expands the synthetic utility of difluorocarbene-involved domino Heck cyclizations and enables the efficient construction of diverse amide-functionalized molecular architectures containing an all-carbon quaternary center.
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ACS Sustainable Chemistry & Engineering
·
2026
·
IF 7.6
Zhengxu Yan,Xujia Cao,Shuai Zhu,Yunyun Gui,Yuan Lin,Linghao Yu,Lijun Liu
Abstract Developing Pd-based catalysts for formic acid (HCOOH) dehydrogenation is of great significance to the advancement of renewable hydrogen utilization. However, traditional Pd surfaces typically display symmetrical electronic and geometrical configurations that suffer from both selectivity issues and CO poisoning phenomena, deteriorating their long-term HCOOH dehydrogenation performance. In this study, we report a bismuth–palladium (BiPd) alloy catalyst with asymmetric electronic and geometric Pd sites that achieved an exceptional H2-evolving turnover frequency (5893.7 h–1) of HCOOH dehydrogenation while maintaining over 96% catalytic activities spanning consecutive 15-round experiments. High-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) and synchrotron X-ray absorption spectroscopy (XAS) characterizations verified the successful construction of BiPd alloys and that Bi components desymmetrized the electronic configuration of Pd sites toward the thermodynamically favored HCOOH dehydrogenation pathway for H2 evolution. On the other hand, in situ diffuse reflectance infrared fourier transform spectroscopy (DRIFTS) and kinetic isotope effect experiments combined with density functional theory (DFT) calculations collectively demonstrated that Bi also diluted Pd ensembles, and the resulting asymmetric Pd architectures reduced the diversity of *CO adsorption configurations on the surface of BiPd alloys, effectively mitigating CO poisoning. This work underscores the critical role of alloying engineering in designing Pd-based catalysts for practically implementing sustainable hydrogen release from liquid organic hydrogen carriers.
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SmartMat
·
2026
·Vol. 7
·期 2
·e70074
·
IF 14.3
Hao Chen,Yuxi Fang,Wanning Zhang,Shunai Che
The slow kinetics and high overpotentials of the oxygen evolution reaction (OER) remains a major challenge for electrocatalytic energy conversion. Spin manipulation has emerged as a promising strategy for enhancing OER performance by modulating the adsorption of intermediates, thereby reducing the reaction energy barrier and accelerating OER kinetics. Herein, we demonstrate that chiral nanostructured Pd films (CNPFs) can enhance OER performance. CNPFs were electrodeposited on a nickel foam substrate using methionine as a symmetry-breaking agent. The optimal CNPFs catalyst achieves a current density of 50 mA∙cm −2 at 1.57 V versus RHE, representing a 180 mV reduction in overpotential compared to achiral Pd films. By varying the electrodeposition time, a series of CNPFs with tunable spin polarization were synthesized. The enhanced OER performance in CNPFs exhibits a positive correlation with spin polarization, primarily due to the spin-polarized electron transfer promoting the formation of triplet oxygen. This work elucidates the fundamental relationship between spin polarization and OER performance, highlighting the critical role of chiral structure in the design of efficient spin-polarized electrocatalysts.
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CHINESE JOURNAL OF CATALYSIS
·
2026
·
IF 17.2
Jiaxiang Qin,Songpei Zhang,Xingju Li,Xintai Chen,Jia Zhao,Xiaoling Mou,Xiangen Song,Li Yan,Ronghe Lin,Yunjie Ding
Precise control over product selectivity in heterogeneous catalysis remains a key challenge due to the complex interplay of structural and electronic factors. Here, we demonstrate delicate tuning of product distribution in 1,3-butadiene semi-hydrogenation by engineering the size and composition of Pd-Ag nanostructures. By systematically decoupling size and electronic effects, we identify critical selectivity descriptors and establish structure-selectivity correlations across both monometallic and bimetallic series. The thresholds of ensemble size and Pd valence state for the formation of distinct products are experimentally determined. Integrating kinetic analysis, chemisorption studies, and density functional theory calculations, we show that increased ensemble size and Ag incorporation weaken 1-butene binding and elevate hydrogenation barriers, enabling selective formation of 1-butene (up to 66%) over thermodynamically favored 2-butenes. These insights reveal the fundamental roles of geometric and electronic modulation in governing selectivity and offer a generalizable framework for the rational design of multifunctional bimetallic catalysts.
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