CATALYSIS TODAY
·
2024
·
IF 5.2
Peng Bai,Yicheng Zhao,Yongdan Li
Photocatalytic N -formylation of amines with CO 2 is a promising strategy to convert CO 2 into value-added chemicals sustainably. In this work, Pd-Bi bimetallic modified ZnO enriched in oxygen vacancies is constructed for photocatalytic CO 2 formylation of benzylamine at room temperature without any reductants. The Pd and Bi sites reduce the band gap energy of ZnO, promote the separation of the photogenerated charge carriers and enhance the adsorption capacity of CO 2 . The yield of N -benzylformamide reaches 31.7 mmol g −1 with a selectivity of 85.3 % after 3-hour radiation in N , N -dimethylformamide (DMF) solvent. The aldehyde group involved in the formylation of benzylamine is derived from the decomposition of DMF, which is regenerated with the aldehyde group coming from the reduction of CO 2 . The decomposition-regeneration cycle of DMF solvent enlarges the reaction region, which is beneficial to the activity and selectivity of the formylation process. The synergistic photocatalytic system shows a good universality. This study provides a new approach to high-efficiency CO 2 utilization and formamide production.
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ENVIRONMENTAL RESEARCH
·
2024
·
IF 7.7
Lan-Ying Liu,Min-Hua Cui,John Justo Ambuchi,Shi-Ming Niu,Xin-Hui Li,Wo-Long Wang,He Liu,Guo-Shuai Liu,Ai-Jie Wang
Electrocatalytic hydrodechlorination (EHDC) is a promising approach to safely remove halogenated emerging contaminants (HECs) pollutants. However, sluggish production dynamics of adsorbed atomic H (H* ads ) limit the applicability of this green process. In this study, bimetallic Pd–Cu@MXene catalysts were synthesized to achieve highly efficient removal of HECs. The alloy electrode (Pd–Cu@MX/CC) exhibited better EHDC performance in comparison to Pd@MX/CC electrode, resulting in diclofenac degradation efficiency of 93.3 ± 0.1%. The characterization analysis revealed that the Pd 0 /Pd II ratio decreased by forming bimetallic Pd–Cu alloy. Density functional theory calculations further demonstrated the electronic configuration modulation of the Pd–Cu@MXene catalysts, optimizing binging energies for H* and thereby facilitating H* ads production and tuning the reduction capability of H* ads . Noteably, the amounts and reduction potential of H* ads for Pd–Cu@MXene catalysts were 1.5 times higher and 0.37 eV lower than those observed for the mono Pd electrode. Hence, the introduction of Cu into the Pd catalyst optimized the dynamics of H* ads production, thereby conferring significant advantages to EHDC reactions. This augmentation was underscored by the successful application of the alloy catalysts supported by MXene in EHDC experiments involving other HECs, which represented a new paradigm for EHDC for efficient recalcitrant pollutant removal by H* ads .
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
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IF 9.7
Zhujiang Wang,Jun Wu,Jieyu Li,Yingxue Fu,Jiaqi Long,Lin Wu,Fenghua Shen,Hao Chen,Kaisong Xiang,Hui Liu,Liyuan Chai
The electrocatalytic reduction of sulfur dioxide (SO 2 ) to hydrogen sulfide (H 2 S) is a promising strategy for efficient sulfur resource utilization. Copper (Cu) catalysts show high selectivity for SO 2 reduction, but their limited hydrogenation capacity restricts H 2 S production. Palladium (Pd), known for its hydrogenation efficiency, was incorporated to overcome this limitation. We synthesized CuPd bimetallic catalysts to enhance hydrogenation efficiency in SO 2 electroreduction. Among these, Cu 67 Pd 33 exhibited superior catalytic performance, achieving a H 2 S partial current density of 201.56 mA·cm −2 (1.08 mmol·cm −2 ·h −1 ), a 120 % increase over Cu and 154 % over Pd. In-situ Fourier-transform infrared spectroscopy (FTIR) and density functional theory (DFT) calculations revealed that Cu primarily catalyzes the reduction of *SOH to *S, while Pd facilitates the activation and dissociation of interfacial water to provide hydrogen and reduces the energy barrier for the conversion of *S to *H 2 S. The synergistic catalysis between Cu and Pd ensures efficient transformation of intermediates and facilitates the conversion of SO 2 to H 2 S. This study highlights a novel strategy for enhancing hydrogenation in SO 2 electroreduction and provides insights into the synergistic mechanisms of CuPd bimetallic catalysts, emphasizing the critical role of interfacial interactions in catalytic performance.
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Journal of Environmental Sciences
·
2024
·
IF 5.9
Zhiqiang Zhang,Wenhang Li,Cailin Zheng,Kunyu Chen,Heliang Pang,Wenxin Shi,Jinsuo Lu
Catalytic reduction of nitrate over bimetallic catalysts has emerged as a technology for sustainable treatment of nitrate-containing groundwater. However, the structure of bimetallic has been much less investigated for catalyst optimization. Herein, two main types of Pd-Cu bimetallic nanocrystal structures, heterostructure and intermetallic, were prepared and characterized using high-resolution transmission electron microscopy (HRTEM), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS). The results show that two individual Pd and Cu nanocrystals with a mixed interface exist in the heterostructure nanocrystals, while Pd and Cu atoms are uniformly distributed across the intermetallic Pd-Cu nanocrystals. The catalytic nitrate reduction experiments were carried out in a semibatch reactor under constant hydrogen flow. The nitrate conversion rate of the heterostructure Pd-Cu nanocrystals supported on α-Al 2 O 3 , γ-Al 2 O 3 , SBA-15, and XC-72R exhibited 3.82-, 6.76-, 4.28-, 2.44-fold enhancements relative to the intermetallic nanocrystals, and the nitrogen and nitrite were the main products for the heterostructure and intermetallic Pd-Cu nanocrystals, respectively. This indicates that the catalytic nitrate reduction over Pd-Cu catalyst is sensitive to the bimetallic structures of the catalysts, and heterostructure bimetallic nanocrystals exhibit better catalytic performances on both the activity and selectivity, which may provide new insights into the design and optimization of catalysts to improve catalytic activity and selectivity for nitrate reduction in water.
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Chem
·
2024
·
IF 19.1
Yang Yang,Guohua Yao,Xiaojuan Zhu,Meiqi Gao,Lili Wang,Shunlin Li,Xuerong Li,Xuezhi Duan,De Chen,Weimin Yang,Ying Wan
Selective hydrogenation of phenol is a sustainable alternative to cyclohexane oxidation for the production of cyclohexanone. However, over-hydrogenation of cyclohexanone to cyclohexanol is thermodynamically favorable, limiting its selectivity. Here, we report an unprecedented cyclohexanone selectivity (>99.9%) in continuous-flow phenol hydrogenation using an electron-deficient Pd catalyst. The Pd atom exists in a unique Pd–N 5 C 4 structure in which it is coordinated with four quasi-planar N atoms and one axial N atom in the first shell and an additional four C atoms in the second shell that lie on the curved surface of a pore in ordered mesoporous carbon. The Pd site has a d charge depletion of 1.18 e that prevents cyclohexanone adsorption, which is therefore exclusively produced. Bonding the Pd atom to a curved plane of carbon atoms is an effective way to control the d charge of Pd and increase its selectivity for the green synthesis of fine chemicals.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
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IF 20.2
Shanhui Zhu,Zexiang Lv,Xiangyu Jia,Jiamin Wang,Xiaoming Li,Mei Dong,Weibin Fan
Hydrogenation of nitroarenes to anilines under mild conditions is attractive from both theoretical and practical viewpoints. Here, high-performance catalyst with layered Pd nanoparticles epitaxially growing on ultrathin MoS 2 nanosheets (Pd/MoS 2 ) were prepared. It shows surprisingly high catalytic activity, selectivity and stability for hydrogenation of various nitroarenes to corresponding anilines; the turnover frequency is one or two magnitudes higher than conventional Pd-based catalysts. Surface sulfur vacancies are formed on MoS 2 nanosheets with low formation energy barrier. These S vacancies provide efficient positions for adsorbing Pd atoms, which enables facile cleavage of N–O bond as result of strong interfacial electron interaction that decreases activation energy by 0.41 eV in comparison with conventional Pd catalysts. In situ spectroscopy and DFT calculation results reveal a dual-site mechanism, in which surface Pd sites adsorb and dissociate H 2 into active H*, and then readily reacts with nearby activated nitroarene to form aniline on interfacial Pd-MoS 2 sites.
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Molecular Catalysis
·
2024
·
IF 3.9
Shengya Ge,Chenzhang Li,Peiyan Bi,Wei Hong
The operation of direct ethylene glycol fuel cells (DEGFCs) to generate electric energy from ethylene glycol rely on the effective electrocatalysts for the ethylene glycol oxidation reaction (EGOR). The fabrication of EGOR electrocatalysts with high activity, high durability and high resistance for corrosion, is essential important for the DEGFCs. Herein, we report a fabrication of Pd nanoparticles immobilized by the Ce-doped ZIF-67-derived carbon (Pd-CeO 2 /ZDC). The Pd nanoparticles are generated by the in-situ reduction reaction between the H 2 PdCl 4 and the Co nanoparticles formed during the ZIF-67 pyrolysis. Owe to the porous structure and N-doping inherited from the ZIF-67, the Pd and CeO 2 nanoparticles show a uniform distribution. Due to the enhanced EGOR electrooxidation kinetic promoted by the ZIF-67-derived support, the multiple-components and structure synergies, the resultant Pd-CeO 2 /ZDC catalyst affords a EGOR current density of 32.4 mA cm -2 , which is higher than the commercial Pd/C as well as the counterpart Pd/ZDC catalyst without CeO 2 . Furthermore, the Pd-CeO 2 /ZDC catalyst also present a better EGOR durability. This work provides a strategy for the design of EGOR catalyst with multiple-components and desired structure, which may inspire the new tactics for controllable design and synthesis of other electrocatalysts for various electrocatalysis.
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International Journal of Oral Science
·
2024
·Vol. 16
·期 1
·1-13
·
IF 10.8
Li Shujin,Feng Tian,Liu Yuantong,Yang Qichao,Song An,Wang Shuo,Xie Jun,Zhang Junjie,Yuan Bifeng,Sun Zhijun
N 1 -methyladenosine (m 1 A) RNA methylation is critical for regulating mRNA translation; however, its role in the development, progression, and immunotherapy response of head and neck squamous cell carcinoma (HNSCC) remains largely unknown. Using Tgfbr1 and Pten conditional knockout (2cKO) mice, we found the neoplastic transformation of oral mucosa was accompanied by increased m 1 A modification levels. Analysis of m 1 A-associated genes identified TRMT61A as a key m 1 A writer linked to cancer progression and poor prognosis. Mechanistically, TRMT61A-mediated tRNA-m 1 A modification promotes MYC protein synthesis, upregulating programmed death-ligand 1 (PD-L1) expression. Moreover, m 1 A modification levels were also elevated in tumors treated with oncolytic herpes simplex virus (oHSV), contributing to reactive PD-L1 upregulation. Therapeutic m 1 A inhibition sustained oHSV-induced antitumor immunity and reduced tumor growth, representing a promising strategy to alleviate resistance. These findings indicate that m 1 A inhibition can prevent immune escape after oHSV therapy by reducing PD-L1 expression, providing a mutually reinforcing combination immunotherapy approach.
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ACS Applied Energy Materials
·
2024
·
IF 5.4
Lanlan Shi,Xiaojun Wang,Feike Zhang,Jingxian Li,Yuanming Liu,Weijie Fu,Shuyun Yao,Shiyu Wang,Kang Ji,Yingjie Ji,Zhiyu Yang,Liwen Zhang,Jiangzhou Xie,Yi-Ming Yan
Palladium metal catalysts have emerged as the preferred choice for alkaline formate oxidation reaction (FOR) due to their high activity. However, their strong binding with adsorbed H (Had) allows Had to occupy the active site, resulting in slow FOR kinetics. Herein, we developed a ZrO2/Pd/C catalyst to decrease the Had binding strength on Pd active sites, thereby enhancing the FOR in alkaline media. Through experimental investigations and density functional theory (DFT) calculations, we elucidated the relationship between the d-band center of Pd and hydrogen binding energy (HBE). Our findings reveal that electron transfer from ZrO2 to Pd, driven by the work function disparity, results in a downshift of the d-band center of Pd. This shift weakens the HBE at Pd active sites, facilitating the desorption of Had intermediates and thereby improving catalytic efficiency. As a result, the ZrO2/Pd/C catalyst demonstrated a 2.8-fold increase in activity over commercial Pd/C, exhibiting a lower peak potential and a significantly higher peak current of 1787 mA mg–1. This work advances our understanding of the interplay between electronic structure and catalytic performance, setting a benchmark for high-performance electrocatalysts in energy conversion technologies.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Jun-Yang Yan,Gui-Ping Cao,Chun-Yan Cao,Peng Gao,Mustapha Sani Shehu,Hui Lv,Alaaddin M. M. Saeed
This work investigated the loading of active metals on monolithic carrier NCNTs@FN through simulation and characterization and found that the active metal (Pd) had a stronger binding with NCNTs and a more uniform dispersion. Meanwhile, the π–π stacking effect between NCNTs and polystyrene (PS) molecules is more significant than that between PS and CNTs, making PS more easily adsorbed. Therefore, the highly active catalyst Pd-NCNTs@FN was prepared. The hydrogenation degree of Pd-NCNTs@FN catalyzed PS reached 92.7%, significantly higher than that of Pd-CNTs@FN (78.1%) under the same conditions. Uniform experiments on PS hydrogenation kinetics were designed. Power law and hyperbolic kinetic models were established, and the corresponding parameters were calculated. From the models, it was found that whether H2 concentration reaches a critical value determines whether H2 pressure affects the hydrogenation rate. In addition, the adsorption of PS is the rate control step in the reaction. The activation energy of Pd-NCNTs@FN catalyzed PS hydrogenation is 47.326 kJ/mol, which is lower than those of other traditional powder heterogeneous catalysts (50–55 kJ/mol), demonstrating the excellent activity of the catalyst.
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CHINESE JOURNAL OF CATALYSIS
·
2024
·
IF 15.7
Ke Huang,Shicheng Yuan,Rongyan Mei,Ge Yang,Peng Bai,Hailing Guo,Chunzheng Wang,Svetlana Mintova
A chlorine-free catalyst consisting of zeolite Y modified with Pd (Pd/NaY) catalyst has been prepared and used in the indirect oxidative carbonylation of methanol to dimethyl carbonate (DMC). The activity and stability of the catalyst were further improved by introducing molybdenum into Pd/NaY using a top-down approach (Pd-Mo/NaY catalyst). The Pd-Mo/NaY catalyst exhibited higher stability compared to the Pd/NaY. A high CO conversion of 97% and DMC selectivity of 80% during a 30-hour catalytic test for the Pd-Mo/NaY were obtained. Furthermore, the incorporation of Mo was found to partially heal the silanols and hinder the aggregation of Pd in the Pd-Mo/NaY catalyst. The interactions between Mo and Pd increased the amount of active Pd 2+ species and enhanced the adsorption of CO reactant on the Pd-Mo/NaY catalyst. The key reaction intermediate of COOCH 3 * was captured by in situ diffuse reflectance infrared Fourier transform spectroscopy . The stabilization of active Pd 2+ species contributed to the enhanced catalytic activity of the Pd-Mo/NaY catalyst in the indirect oxidative carbonylation of methanol to DMC reaction.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yangzi Zheng,Jiapeng Huang,Ruiyun Guo,Tianou He,Yanan Li,Yaming Liu,Weicong Wang,Qi Zhan,Shangdong Ji,Mingshang Jin
The formic acid oxidation reaction (FAOR) in direct formic acid fuel cells (DFAFCs) relies heavily on the use of Pd catalysts. To improve the performance of DFAFCs, it is crucial to develop highly active and stable Pd catalysts for FAOR. In this work, we demonstrate a novel approach to enhance the electrocatalytic activity and stability of Pd nanocatalysts by incorporating a palladium phosphide (Pd-P) interlayer. The introduction of the Pd-P interlayer can facilitate electron transfer and enhance the vacancy formation energy of the active Pd sites on the surface of Pd@Pd-P@Pd nanocrystals. As a result, the Pd@Pd-P@Pd catalyst can exhibit exceptional long-term durability, with a mass activity of 4.56 A mg -1 Pd and a specific activity of 28.06 mA cm −2 towards FAOR, which are 11.5 and 18.1 times higher than those observed for the commercial Pd/C catalyst, respectively. By leveraging the unique properties of the interlayer in Pd nanocatalysts, this work opens up a promising pathway for enhancing the performance of catalysts in sustainable energy conversion systems.
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