ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2026
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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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CHINESE JOURNAL OF CATALYSIS
·
2026
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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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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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JOURNAL OF ORGANIC CHEMISTRY
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2026
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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
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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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CHEMICAL ENGINEERING JOURNAL
·
2025
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IF 13.2
Hao Chen,Quanzheng Deng,Tianwei Ouyang,Wanning Zhang,Bin Liu,Lu Han,Shunai Che,Yuxi Fang
The electrochemical reduction of NO x to ammonia presents a dual solution to both energy and environmental crises. Despite substantial progress in developing strategies to enhance the efficiency, the design of catalysts and the elucidation of the reaction mechanism remain significant challenges. Herein, we propose that the spin polarization of chiral nanostructured Pd films (CNPFs) can facilitate the formation of triplet 3 NOH by regulating the parallel electron spin alignment. Additionally, the helical lattice distortion of nanostructures can decrease reaction energy of adsorbed intermediates, thereby triggering multiple proton-coupled electron transfer steps to promote the generation ammonia. The CNPFs with helical lattice distorted nanoflakes were fabricated via electrodeposition using methionine as a symmetry-breaking agent. In the electrocatalytic reduction of nitrite to ammonia, the CNPFs achieved a maximum Faradaic efficiency (FE) of 97.6 % for NH 3 at −0.6 V vs. reversible hydrogen electrode. Ammonia was not detected in the nitrite-free electrolyte solution, indicating a direct correlation between the presence of nitrite in the solution and the production of ammonia. This work elucidates the critical roles of spin polarization and helical lattice distortion in the nitrite electroreduction reaction, revealing the underlying mechanisms of reactions involving triplet intermediates.
研究领域:
材料科学
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电催化
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环境科学
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Journal of Materials Chemistry C
·
2025
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IF 5.1
Huifeng Yuan,Jianting Li,Wei-Feng Rao,Shuo Qu,Guiqi Gao,Hou Tiancheng,Yaodong Yang
The synergistic coupling of piezoelectric catalysis and photocatalysis can significantly enhance hydrogen production efficiency. However, developing high-performance catalysts with both high piezo/photo-response remains a key challenge. In this study, Palladium nanocrystals (Pd-NCs) have been deposited on the surface of SrBi4Ti4O15 (SBTO), resulting in the successful construction of an efficient hydrogen evolution catalyst based on the synergistic effect of piezo-photocatalysis.Under simultaneous illumination and ultrasound, SBTO-Pd-10% exhibited a hydrogen evolution rate of 27.6 mmol g -1 h -1 , representing an eleven-fold enhancement relative to pure SBTO. The enhanced performance can be attributed to the incorporation of Pd-NCs, which extends the visible light absorption spectrum of SBTO-Pd composite, improves conductivity, and introduces additional catalytic sites, thereby promoting efficient charge carrier separation. Additionally, ultrasonic effect induced an internal piezoelectric field that further inhibited photogenerated carrier recombination, resulting in a significant enhancement of performance. This study reveals the synergistic catalytic mechanism of coupled piezo-photocatalytic system, which provides a feasible pathway for the future design of highly efficient hydrogen production catalysts.
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GREEN CHEMISTRY
·
2025
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IF 9.2
Aichun You,weixian Lian,Xian liang Fu,Yuge Fan,Jinni Shen,Xuan Zhao,Li Zhu,Fan Tian,Man Xu
A highly efficient continuous-flow catalytic system for the ambient hydrogenation of nitroarenes to arylamines has been developed using a 1 wt.% Pd catalyst supported on robust, chemically stable SiC nanowires (Pd/SiC NWs). This system achieved 97% conversion and 98% selectivity for converting 4-nitrophenol (4-NP) to 4-aminophenol (4-AP) within 5 minutes using NaBH₄ as a hydrogen donor. A pseudo-first-order reaction rate constant of 0.753 min⁻¹ was determined, which is 4.5 times faster than that observed in a batch reaction system and significantly surpasses rates achieved with Pd supported on other common carriers (activated carbon, silica, alumina) and other noble metals (Pt, Au, Ag) supported on SiC NWs. The reaction system demonstrated high stability and a broad substrate scope for various substituted nitroarenes. The high catalytic activity is attributed to the synergistic interaction between the Pd catalyst and the SiC NWs substrate, which enhances the dissociation of NaBH₄ to produce H* and facilitates the subsequent transfer of H* to the substrate, resulting in the formation of mobile and reactive Si-H* species. This process promotes the hydrogenation of the preferentially adsorbed 4-NP on SiC NWs. Furthermore, the forced mass transfer and the uniformity of the reaction microenvironment, which prevent back-mixing of reactants and intermediates in the flow system, ensure the sequential hydrogenation of the -NO2 group via the Haber’s direction route mechanism, with nitroso as the primary intermediate. This research offers a promising approach for the efficient and convenient synthesis of arylamines.
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Frontiers in Chemistry
·
2022
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IF 5.545
He Limin,Wang Yangdong,Wang Can,Liu Zhicheng,Xie Zaiku
The hydrogenation of 4-carboxylbenzaldehyde over Pd catalysts is a crucial process during the production of pure terephthalic acid. Herein, ZIF-8 derived carbon materials (NC) with adjustable N types were synthesized and used as the supports of Pd catalysts. Pd supported on NC with 50.5% of pyridinic N exhibited best hydrogenation activity with a TOF value of 4.1 min−1. The microstructures of NC support and electronic structures of Pd in Pd/NC were investigated by techniques such as XRD, N2 physisorption, XPS, H2-O2 titration and TEM. The nitrogen species in CN surface not only can adjust chemical state and dispersion of Pd nanoparticles (NPs), but also promote the adsorption and activation capability of H2 molecular. Besides, the ratio of Pd0/Pd2+ and Pd dispersion were closely correlated with pyridinic nitrogen content. The improvement in hydrogenation activity and stability of Pd/CN catalyst in relative to Pd/C were ascribed to the synergistic effect of pyridinic nitrogen and active site Pd0.
研究领域:
催化化学
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材料科学
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Advanced Science
·
2025
·
IF 14.1
Manman Tan,Chengyu Shi,Guangyi Chi,Xinwan Su,Fangzhou Liu,Linyu Zhu,Guangqian Cheng,Xiangyi Chen,Meng Yu,Yijian Chen,Ying Wang,Yu Chen,ShuLing Yan,Wenfei Wu,Qingfeng Yan,Jianzhong Shao,Kai Wang,Xiangrui Liu,Min Zhou,Aifu Lin
Peptide-based therapeutic strategies offer considerable potential for tumor immunotherapy but suffer from poor systemic bioavailability, rapid plasma clearance, and limited tumor-targeting efficiency. To address these challenges, a biomimetic, photothermal-responsive liposomal delivery system was developed that enables precise delivery of immunotherapeutic peptides while enhancing the synergistic effects of photothermal therapy. This system enhances peptide stability through fluorination, disrupts post-translational modifications of PD-L1, and promotes its degradation, thereby amplifying the anti-tumor immune response. The carrier core consisted of thermosensitive 1,2-dipalmitoyl-sn-glycero-3-phosphocholine (DPPC) liposomes loaded with the low-toxicity photosensitizer indocyanine green (ICG), which facilitated controlled peptide release via the photothermal effect. Simultaneously, mild photothermal stimulation induced immunogenic cell death (ICD), further strengthening anti-tumor immunity. To enhance tumor targeting, extend systemic circulation time, and improve drug accumulation at tumor sites, the carrier surface was coated with a platelet membrane, which increased biocompatibility and promoted immune evasion. Notably, in vivo studies demonstrated that the developed bioengineering platform significantly suppressed tumor growth in both solid and diffuse malignant tumors while inducing persistent immune memory, thereby facilitating long-term anti-tumor immune responses. Collectively, this approach establishes a novel framework for integrating peptide drug delivery with photothermal therapy, offering a promising strategy for advancing tumor immunotherapy.
研究领域:
癌症免疫治疗
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药物递送系统
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纳米医学
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光热治疗
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生物工程
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分子生物学
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-8
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IF 15.7
Deng Peilin,Xu Yueshan,Wu Daoxiong,Liang Ying,Zhang Xue,Wang Zhitong,Li Jing,Tian Xinlong
Pd catalysts demonstrate remarkable activity and selectivity for the direct oxidation methane-to-methanol (DOMM) under mild conditions. However, understanding the structure–performance relationship is challenging because Pd catalysts used in existing studies have complex polycrystalline structures. In this work, well-defined Pd nanocrystals with controlled morphologies are synthesized and used as model systems to investigate the origins of the observed structure-activity differences. Our findings indicate that DOMM activity is primarily governed by crystal facet type rather than nanocrystal size. The lower d -band center of the Pd {111} facet weakens the adsorption strength of critical intermediates, including *O 2 and *OH species, promoting H 2 O 2 generation and CH 3 OH formation, respectively. Consequently, {111}-dominated octahedral Pd nanocrystals achieve an exceptional CH 3 OH yield of 201.8 mmol·g Pd −1 ·h −1 , three times higher than that of their {100}-dominated hexahedral counterparts. These results provide key insights into the structure-dependent behavior of Pd catalysts and pave the way for designing high-performance catalysts for DOMM.
研究领域:
催化
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纳米技术
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化学反应工程
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材料科学
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环境化学
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
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IF 8.3
HongWei Li,Peng Guo,BoYu Huang,Dong Ji,GuiXian Li,XinHong Zhao
Rational modulation of metal-support interaction (MSI) is pivotal yet challenging for developing high-performance electrocatalysts. Herein, we demonstrate a promoter engineering strategy to precisely tune the N configuration in ZIF-8-derived carbon supports for boosting Pd-catalyzed methanol oxidation reaction (MOR). Structurally diverse organic promoters (urea, dicyandiamide, sucrose, xylitol) impregnated in ZIF-8 pores regulate pyrolysis behavior, yielding N-doped carbons with optimized porosity, graphitization, and N-configuration. Among them, urea-modified support (NC–U) demonstrates the highest surface area (925 m 2 g −1 ) and graphitic-N content (40.4 %), facilitating uniform dispersion of ultrasmall Pd nanoparticles (2.71 nm) and electron transfer to enrich metallic Pd 0 (75.2 %). The resulting Pd/NC-U delivers exceptional MOR activity (5570.7 mA·mg −1 Pd ) and stability (87.4 % retention after 500 cycles), outperforming unmodified Pd/NC by 1.32-fold. Besides, operando SERS reveals a CO-free pathway on all catalysts, with Pd/NC-U initiating HCO 3 − /CO 3 2− formation at the lowest potential (0.4 V vs. RHE). This work establishes promoter-mediated N-configuration control as a robust route to tailor MSI for efficient alcohol electrooxidation.
研究领域:
材料科学
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电催化
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纳米技术
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能量转换
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