SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
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.
✓ 已验证
产品关联
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
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.
✓ 已验证
产品关联
DOI
高影响因子
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.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
·
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.
✓ 已验证
产品关联
DOI
高影响因子
SURFACE AND INTERFACE ANALYSIS
·
2022
·Vol. 55
·期 4
·279-287
·
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.
✓ 已验证
产品关联
DOI
高影响因子
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.
✓ 已验证
产品关联
DOI
高影响因子
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.
✓ 已验证
产品关联
DOI
高影响因子
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.
✓ 已验证
产品关联
DOI
高影响因子
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.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING RESEARCH & DESIGN
·
2018
·
IF 2.795
Hao Feng,Biao Zhang,Xun Zhu,Rong Chen,Qiang Liao,Ding-ding Ye,Jian Liu,Ming Liu,Gang Chen
Microreactors are promising for fine chemistry and value-added chemical synthesis, but the small dimension places significant challenges in catalyst layer fabrication. Meanwhile, enhancing catalyst dispersion to obtain smaller particle size are of great interests. We proposed a multilayered Pd nanocatalysts with nano-bulge structure inside a microreactor for multiphase catalytic reaction. The unique bulged nanostructure can provide more accessible sites for precursor (PdCl 4 2− ) adsorption, and extend the available area to reduce the Pd nanoparticle size. Experimental results show rugged Pd catalyst layer with the nano-bulge structure was prepared, and both the precursor utilization rate and Pd nanocatalysts dispersion were enhanced, resulting in 35.4% higher catalyst loading and 4-fold smaller particle size. Benefitting from these advantages, compared with conventional Pd coated polydopamine catalyst layer, the proposed multilayered Pd nanocatalyst can significantly intensify the reaction rate and obtain an order of magnitude longer durability in nitrobenzene hydrogenation. This versatile and convenient fabrication method can be used in fabricating high performance and durable catalyst layers in microreactors.
✓ 已验证
产品关联
DOI
高影响因子
POLYMER BULLETIN
·
2019
·Vol. 77
·期 2
·1003-1014
·
IF 1.858
Zhang Xinxin,Shi Haoyan,Chi Quan,Liu Xixi,Chen Lianqing
Cellulose-supported on Pd nanoparticles (Pd/cellulose) were successfully prepared by chemical reduction technique and characterized by various experimental tools. The Pd/cellulose catalyst was found to effectively promote the oxidation of glucose into gluconic acid under mild conditions. The base played a crucial role in the oxidation of glucose into gluconic acid. Glucose was fully converted at room temperature after 3 h by the use of stoichiometric amount of Na 2 CO 3 to neutralize gluconic acid, and gluconic acid was obtained in a high yield of 91.2%. The catalyst was recovered from product and reused up to five times without significant loss in its catalytic activity.
✓ 已验证
产品关联
DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2018
·
IF 5.667
Wenchi Zhang,Xiangheng Niu,Suci Meng,Xin Li,Yanfang He,Jianming Pan,Fengxian Qiu,Hongli Zhao,Minbo Lan
In this work, we proposed a new and facile strategy for the high-performance colorimetric detection of Ag + based on the tunable peroxidase-like activity of Pd nanoparticles (NPs) mediated by histidine (His). Bare Pd NPs possess intrinsic catalytic ability to trigger the oxidation of colorless 3,3′,5,5′-tetramethylbenzidine (TMB) to blue TMBox in the presence of H 2 O 2 . After being decorated by His, the formed His-Pd nanozyme exhibits significantly improved mimetic activity due to its favorable physicochemical characteristics including smaller size, interactions between Pd and His, and better hydrophilicity, and such that an enhanced TMB color reaction is observed. When Ag + exists, it is able to despoil the His modifier from the His-Pd surface via the specific interaction between Ag + and His, resulting in the bald Pd again with weak activity. With this principle, highly sensitive determination of Ag + in a linear scope of 30–300 nM was achieved with a limit of detection down to 4.7 nM. In addition, the colorimetric sensor based on the tunable enzymatic activity of nanosized Pd adjusted by His could provide excellent selectivity for Ag + sensing against common interferents. Reliability of the strategy for practical detection of Ag + was also demonstrated.
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）