APPLIED SURFACE SCIENCE
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2023
·
IF 6.7
Di Wang,Hongcen Yang,Shuhao Tian,Guo Liu,Ying Wang,Xiao Sun,Zhixia Wang,Juan Hou,Fei Ma,Shanglong Peng
Hydrogen energy is regarded as the clean energy alternative for fossil energy. Hydrogen evolution reaction (HER) is a sustainable way for the production of hydrogen energy. However, commercial platinum (Pt) catalysts for HER are expensive and scarce, which will not fully meet the demand of the future market. Therefore, scientists have been actively exploring alternatives to Pt-based catalysts. Studies have shown that palladium (Pd) and Pt have similar catalytic activity in HER. Small molecular Pd nanoclusters can be used as a perfect HER activity center. Herein, anchoring of Pd nanoclusters (Pd NCs) on sulfur-vacancy-enriched ZnIn 2 S 4 nanosheets (Pd/ZIS-T) has been successfully achieved. The zeta potential value for ZnIn 2 S 4 is −59.9 mV, indicating that the surface of ZnIn 2 S 4 is abundant negatively charged in deionized water, thus providing plentiful anchoring sites to absorb Pd 2+ . The results show that the synergistic effect of Pd NCs and sulfur vacancies will endow the obtained catalyst with excellent electrocatalytic activity and stability. It also managed to reducing costs by reducing noble metal content. In particular, the Pd/ZIS-T electrocatalyst with excellent performance delivered low overpotential of 25 mV at 10 mA cm −2 and small Tafel slope of 33 mV dec -1 in acidic electrolyte.
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Asian Journal of Organic Chemistry
·
2023
·Vol. 12
·期 7
·e202300216
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IF 2.7
Yi-Ying Zhuang,Xiao-Chao Chen,Kai-Chun Zhao,Guo-Sheng Zhang,Yu-Fen Xie,Yong Lu,Ye Liu
Graphical Pd-catalyzed anti -Markovnikov hydrocarboxylation of vinylarenes with formic acid free of auxiliary additive has been reported. This work was financially supported by the National Natural Science Foundation of China (Nos. 22172052 and 21972045), and the Research Funds of Happiness Flower ECNU (2022ST2203).
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Journal of Materials Chemistry A
·
2023
·Vol. 11
·期 19
·10222-10227
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IF 11.9
Ziqiang Wang,Guanghui Yang,Pengjun Tian,Kai Deng,Hongjie Yu,You Xu,Xiaonian Li,Hongjing Wang,Liang Wang
Water electrolysis for hydrogen production consumes abundant electronic energy owing to the sluggish oxygen evolution reaction (OER), so the integration of the hydrogen evolution reaction (HER) with thermodynamically more favorable oxidation reactions is a promising strategy for energy-efficient hydrogen production. Herein, we propose the epitaxial confinement of rhodium nanoparticles (NPs) to palladium metallene (Rh/Pd metallene) for hydrogen production assisted by the hydrazine oxidation reaction (HzOR). The two-dimensional structure of Rh/Pd metallene provides sufficient active sites as well as a rapid charge transfer rate. The interface of Pd metallene with Rh NPs ensembles to modulate the electronic state, thus optimizing the adsorption energy of reaction intermediates. The Rh/Pd metallene exhibits splendid HER and HzOR activities, with overpotentials of 59 and 7 mV at 10 mA cm−2, respectively. In the two-electrode construction of a hydrazine oxidation-assisted water splitting system, the Rh/Pd metallene only needs a low overpotential of 0.19 V to produce hydrogen at a current density of 100 mA cm−2. This research offers a viable approach for designing nanosheet/nanoparticle heterojunction as an attractive modular platform for energy-saving hydrogen production.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Jianhui Xu,Xin Fu,Yufeng Liu,Yunfei Zhang,Shenggui Chen,Dan Li,Chunhui Zhang,Jiale Gao,Yibo Fu
Electrocatalytic hydrodechlorination technology provides an attractive strategy to effectively eliminate the biotoxicity of halogenated organic pollutants (HOPs). Herein, we demonstrated a highly dispersed Pd loaded on blue TiO 2 nanotube arrays (Pd x -BTNA) cathode that can achieve efficient dechlorination and detoxification toward florfenicol (FLO). Characterization results indicated that strong interaction between Pd and BTNA was achieved through Pd-O bonds, which facilitated the electron transfer rate. Pd x -BTNA significantly outperformed other cathodes (i.e., BTNA, Pd x -TNA and Pd x -Ti) in the electrocatalytic dechlorination of FLO due to enhanced utilization of active H*. The dechlorination performances of FLO well followed the pseudo-first-order kinetic, and the reaction constant rate on Pd x -BTNA cathode (0.035 min −1 ) was 17.5, 1.94, 7.0 times higher than that on BTNA, Pd x -TNA and Pd x -Ti cathodes, respectively. Quenching experiments and electrochemical characterization indicated that both direct electron transfer and indirect reduction process mediated by H* were involved in the dechlorination of FLO. The optimal dechlorination efficiency of 98.79% was obtained by Pd x -BTNA cathode within 120 min at 1 mM PdCl 2 , applied cathode potential of −1.2 V. In addition, Pd x -BTNA exhibited superior stability and durability with almost no Pd leaching (0.0011 mg/L) during five dechlorination cycles. Our research proposed a novel strategy to design low noble Pd-loaded cathode material for efficient dechlorination and detoxification of HOPs.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
·
IF 5.2
Jianguo Yu,Zehui Yu,Yunling Jia,Ting Ran,Ming Song,Yanshuang Zhang,Qing Wang,Yuning Qu,Lili Wang
Direct alcohol fuel cells' performance is significantly affected by the phase and composition of the catalyst, thereby the development of high-performance alcohol oxidation catalysts is essential. In this study, PVA preparation was used for the first time to create PdCu core-shell nanoflowers with a high electrochemically active surface area and a potent synergistic effect. Notably, the presence of PVA causes Pd and Cu nanoparticles with different reduction rates to form a core-shell structure, and the Pd nanoparticles continue to migrate regularly under the action of PVA, forming a flower-like morphology with a high degree of branching. Cu@Pd 22.3 catalyst exhibited 13 times higher catalytic performance (4353.04 mA mg Pd −1 ) than Pd/C (334.09 mA mg Pd −1 ) in ethylene glycol oxidation reaction. The Cu@Pd 22.3 catalyst also exhibits higher stability than commercial Pd/C in stability tests lasting up to 20,000 s. This core-shell combination and highly branched structural design result in more active sites for fast ion adsorption/desorption,offering an original method to improving the activity and endurance of polyol oxidation.
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Nano Research
·
2023
·
IF 9.9
Ye Zichen,Li Yun,Li Jingchao,Hu Xinyan,Zheng Jinyang,Zhang Gongxin,Xiang Sijin,Zhu Tianbao,Guo Zhide,Chen Xiaolan
Lactic acid (LA) plays a major role in the occurrence, development, and spread of cancer. Enlightened by its high accumulation in tumor site, a novel lactate oxidase (LOD) conjugated two-dimensional Pd@Ir nanoplatform (Pd@Ir-LOD, PIL) was fabricated to combine cascade reaction with photothermal for tumor therapy. In detail, the overexpressed LA in tumor microenvironment (TME) was a key factor to activate the PIL-based cascade reaction: (1) Plenty of H 2 O 2 could be generated from LA by the catalysis of LOD with O 2 ; (2) potent OH was produced from H 2 O 2 due to the peroxidase (POD)-like activity of PIL; (3) meantime, PIL’s catalase (CAT)-like activity could decompose part H 2 O 2 into O 2 to achieve the purpose of LA cyclic oxidization. Moreover, the reduced glutathione (GSH) scavenging capability of PIL might protect the produced reactive oxygen species (ROS) from being cleared to further improve the cascade therapeutic effect. More importantly, PIL had excellent photothermal conversion efficiency (37.35%) and manifested a surprising temperature rising effect in tumor. Taken together, the decreasing LA concentration, accumulation of high-toxic ROS, the depletion of GSH together with the higher intra-tumoral temperature potently enhanced in vivo antitumor therapy. Therefore, a promising therapeutic tactic based on PIL integrating endogenous LA consumption, chemodynamic therapy (CDT), and photothermal therapy (PTT) has been put forward.
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JOURNAL OF CATALYSIS
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2023
·
IF 7.3
Hao Xu,Hao Li
Constructing heterogeneous catalysts with high efficiency and stability to achieve biomass HDO under comparatively mild conditions is an arduous challenge. Crystal phase of metal oxides supports could affect the geometric and electronic properties, causing the variation of catalytic performance. Herein, a series of Pd/Nb 2 O 5 catalysts of pseudohexagonal crystal phase (Nb 2 O 5 -TT), orthorhombic phase (Nb 2 O 5 -T) and monoclinic phase (Nb 2 O 5 -H) are prepared through regulating the annealing temperature. Impressively, Pd/Nb 2 O 5 -T catalyst showed amazing catalytic performance of 100% conversion and 98.9% selectivity of 2-methoxy-4-methylphenol (MMP) at room temperature (25℃) within 30 min, superior than Pd/Nb 2 O 5 -TT, Pd/Nb 2 O 5 -H and other Pd-based catalysts that had been reported. Besides, the Pd/Nb 2 O 5 -T perform robust stability and maintain its high activity after ten times recovery experiment. This catalytic system is also suitable for different kinds of aldehydes compounds at room temperature, exhibiting the high activity and selectivity towards deoxygenated products. Based on the characterizations and experimental validations, it has confirmed that the strong metal-support interaction (SMSI) effect generates via electron transfer between Pd species and Nb 2 O 5 -T support, where in situ reduction of PdO occurred during the reaction, generating active interfacial Pd-O-Nb sites and accelerating the breaking of C-O bonds. The insights of this work provide a guiding direction for the future design of highly selective heterogeneous catalysts by crystal phase modulation engineering.
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SURFACE AND INTERFACE ANALYSIS
·
2022
·Vol. 55
·期 4
·279-287
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IF 1.702
Mengnan Qu,Bin Zhang,Yandong Wang,Yanqing Lv,Jianwei Ge,Yaxin Wu,Min Yan,Lei Shen,Jinmei He
Wettability is an important property of solid surfaces, superwetting materials can be prepared by controlling the surface morphology and surface energy. In recent years, superwetting materials have been researched and used widely in the fields of self-cleaning, anti-fogging, microfluidics, and oil–water separation, but few studies about superwetting materials in chemical reactions have been conducted. In the multiphase reaction, the low solubility and diffusion rate of gas lead to inferior mass transfer, which restricts the reaction kinetics and reduces the reaction rate. Therefore, it may be a breakthrough to make the solid surface obtain underwater superaerophilicity. In this paper, 1H,1H,2H,2H -perfluorooctyltriethoxysilane (POTS) with low surface energy was constructed on the palladium-carbon nanotubes (Pd-CNTs), as-prepared Pd-CNTs/POTS composite has excellent hydrophobicity and underwater superaerophilicity. When Pd-CNTs/POTS composite was utilized in the catalytic hydrogenation, Pd-CNTs/POTS composite shows higher catalytic activity than Pd-CNTs; the higher catalytic performance is attributed to the underwater superaerophilicity, which enables gaseous hydrogen to rapidly accumulate on the surface of material, increasing the gas–liquid–solid reaction interface formed. The strategy looks forward to providing a new way for developing novel and efficient heterogeneous catalysts and reaction systems.
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ACS Sustainable Chemistry & Engineering
·
2019
·
IF 6.97
Yuwei Shen,Dingchang Shi,Liangbin Liu,Fan Liao,Wenxiang Zhu,Mingwang Shao
The electrocatalytic activity is closely associated with the electronic structure of catalysts. Electron-deficient palladium (Pd) has been proved to show better oxygen reduction reaction performance than the electrophilic one due to the downshift of the d-band center. In this work, Pd nanoparticles are uniformly dispersed in F, N-doping graphene with the assistant of silicon nanowires and hydrofluoric acid (Pd/F, N-doping G). A strong interaction between the metal and doped-graphene leads to the electron-deficiency of the modified Pd, which is beneficial for obtaining proper adsorption energy of oxygen species. The as-prepared Pd/F, N-doping G-3 catalyst shows a four-electron oxygen reduction pathway with large half-wave potential of 0.87 V and high onset potential of 0.99 V in 0.1 M KOH. In addition, the Pd/F, N-doping G-3 based zinc-air battery exhibits an open potential of 1.40 V and a high power density of 229 mW·cm–2.
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ACS Catalysis
·
2019
·
IF 12.221
Yong Xu,Wenyi Bian,Qi Pan,Mingyu Chu,Muhan Cao,Youyong Li,Zhongmiao Gong,Rui Wang,Yi Cui,Haiping Lin,Qiao Zhang
The development of highly selective catalysts has been remarkably relying on the understanding of catalytic active sites. Pd-catalyzed semihydrogenation of propyne has been a focus of research with industrial applications toward the production of polymer-grade propylene. In this work, combining density functional theory (DFT) calculations and experimental observations, we propose that, different from the existing debates where the formation of palladium carbide (Pd–C) species or specific facets of Pd nanoparticles are critical, the apexes of Pd (111) octahedrons are the active sites for highly selective propyne semihydrogenation. The propylene selectivity on Pd octahedrons can be ascribed to site-selective propyne adsorption on the apexes prior to reactions and subsequent difficult to access intermediate states toward overhydrogenation. To reveal the active sites of Pd, propyne semihydrogenation was performed on shaped-Pd nanoparticles with designed exposed facets: e.g., (111) and (100) facets. Of practical importance, the propyne conversion and propylene selectivity exceed ∼94% and ∼96% on Pd octahedrons, respectively, at low temperature (35 °C) and atmospheric pressure. In addition, more control experiments have been performed to verify the effects of apexes of Pd octahedrons on propylene selectivity. It is shown that the propylene selectivity decreases to ∼50% when the apexes of Pd octahedrons are gradually removed. The experimental observations have further confirmed that the apexes of Pd octahedrons can be used as the active sites for propyne semihydrogenation, which is in good agreement with the results from theoretical calculations. This work may not only reveal the active sites of Pd nanoparticles for selective semihydrogenation of propyne but also open an avenue for designing highly active and selective catalysts in the chemical industry.
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JOURNAL OF CATALYSIS
·
2019
·
IF 7.723
Da Yang,Lei Liu,Dong-Liang Wang,Yong Lu,Xiao-Li Zhao,Ye Liu
A series of novel multi (bi-/tri-/tetra-)-dentate phosphines with good robustness against water and oxygen were synthesized and fully characterized. It was found that the developed ionic tri-dentate phosphine ( L2′ ) enabled Pd-catalyzed alkoxycarbonylation of alkynes most efficiently while H 2 O was used as an additive instead of acid. As for L2′ , its unique steric configuration with two types of potential P-P chelation modes (P⋯P distance of 4.31 Å and 4.36 Å respectively) to Pd-centre rendered the corresponding Pd-catalyst high activity and good stability for alkoxycarbonylation of alkynes. The in situ FT-IR analysis also verified that the formation and stability of Pd–H active species were greatly facilitated with the presence of L2′ as well as H 2 O additive. In addition, as an ionic phosphine, L2′ based PdCl 2 (MeCN) 2 system immobilized in RTIL of [Bmim]NTf 2 could be recycled for 7 runs without obvious activity loss or metal leaching.
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CRYSTENGCOMM
·
2019
·Vol. 21
·期 11
·1772-1779
·
IF 3.382
Zheng Deng,Xinsheng Peng,Yu-Jia Zeng
Modulators were frequently employed to synthesize UiO-66 with improved crystallinity, enhanced porosity, and controlled size and morphology. However, little attention was paid to the functionality of modulators themselves. We showed that ferrocenecarboxylic acid (FcCOOH) was not only an efficient modulator for UiO-66 synthesis but also endowed UiO-66 with redox properties. FcCOOH significantly reduced the size of UiO-66 from 400 nm intergrown crystals into 50 nm individual ones, and at the same time remarkably improved their crystallinity, micro-pore volume (0.56 cm3 g−1), and BET surface area (1364 m2 g−1). In addition, FcCOOH in UiO-66 served as a reducing agent for in situ incorporation of Pd nanoparticles into UiO-66 under mild conditions and was used as an efficient heterogeneous catalyst for the Suzuki–Miyaura reaction.
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