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SENSORS AND ACTUATORS B-CHEMICAL · 2024 · IF 8

Chemiresistive detection of H2 at near room temperature by porous In2O3 nanotubes co-sensitized with La-dopant and Pd-modifier

Xuping Li,Yanwei Li,Xingtang Xu,Xiaohua Wang,Guang Sun,Bo Zhang,Yan Wang,Jianliang Cao

Metal oxide semiconductor (MOS)-based hydrogen (H 2 ) sensor that can work at room or near room temperature has attracted an increasing concern owing to its potential application in hydrogen storage and utilization. Herein, a co-sensitization strategy by La doping and Pd decoration is proposed to realize the detection of H 2 at near room temperature (50 °C) on In 2 O 3 porous nanotubes (PNTs). The In 2 O 3 PNTs were prepared via a solvothermal method and then sequentially doped with La 3+ and decorated with Pd nanoparticles via an immersion, freeze-drying and calcination route and a chemical reduction method, respectively. The results of gas-sensing measurements indicated that after a compositional evolution from In 2 O 3 to La-doped In 2 O 3 (La-In 2 O 3 ) and Pd-decorated La-In 2 O 3 (Pd/La-In 2 O 3 ), the fabricated H 2 sensor showed a higher sensitivity at lower operating temperature. At a near room temperature of 50 °C, the response of the best Pd/La-In 2 O 3 sensor to 50 ppm H 2 was as high as 8.34, increasing about 4.85, 1.20 and 1.15 folds compared to the In 2 O 3 (1.72 at 160 °C), La-In 2 O 3 (6.97 at 150 °C) and Pd/In 2 O 3 (7.24 at 80 °C) sensors, respectively. The sensitization effects and mechanism of La dopant and Pd modifier as well as their synergistic effects were discussed in detail.

CAS / MDL: 7647-10-1
研究领域: 材料科学 · 化学
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Green Energy & Environment · 2023 · IF 13.3

Construction of Pd-doped RuO2 nanosheets for efficient and stable acidic water oxidation

Yibo Liu,Xing Hu,Chenxi Liu,Shan Zhu,Kezhu Jiang,Feng Liu,Shijian Zheng

RuO 2 has been considered a potential alternative to commercial IrO 2 for the oxygen evolution reaction (OER) due to its superior intrinsic activity. However, its inherent structure dissolution in acidic environments restricts its commercial applications. In this study, we report a novel Pd-doped ruthenium oxide (Pd–RuO 2 ) nanosheet catalyst that exhibits improved activity and stability through a synergistic effect of Pd modulation of Ru electronic structure and the two-dimensional structure. The catalyst exhibits excellent performance, achieving an overpotential of only 204 mV at a current density of 10 mA cm −2 . Impressively, after undergoing 8000 cycles of cyclic voltammetry testing, the overpotential merely decreased by 5 mV. The PEM electrolyzer with Pd 0.08 Ru 0.92 O 2 as an anode catalyst survived an almost 130 h operation at 200 mA cm −2 . To elucidate the underlying mechanisms responsible for the enhanced stability, we conducted an X-ray photoelectron spectroscopy (XPS) analysis, which reveals that the electron transfer from Pd to Ru effectively circumvents the over-oxidation of Ru, thus playing a crucial role in enhancing the catalyst's stability. Furthermore, density functional theory (DFT) calculations provide compelling evidence that the introduction of Pd into RuO 2 effectively modulates electron correlations and facilitates the electron transfer from Pd to Ru, thereby preventing the over-oxidation of Ru. Additionally, the application of the two-dimensional structure effectively inhibited the aggregation and growth of nanoparticles, further bolstering the structural integrity of the catalyst.

CAS / MDL: 7758-02-3
研究领域: 材料科学 · 电化学
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SENSORS AND ACTUATORS B-CHEMICAL · 2024 · IF 8

Surface engineering of 1D Na-doped Pd/WO3 nanorods for chemiresistive H2 sensing

Xuan-Yu Yang,Hao-Nan Chen,Li-Juan Yue,Fei-Long Gong,Ke-Feng Xie,Shi-Zhong Wei,Yong-Hui Zhang

The design of novel functional nanostructures for advanced chemical engineering field is of great importance. In this work, Pd-modified Na-doped WO 3 nanorods are rationally designed for rapid and detection of hydrogen, which is a green and clean energy in modern industry. Notably, and H + as well as citrate ions play an important role in the formation of 1D nanorods, and the morphology formation mechanism is explored. Here, inspired by the novel Pd-modified Na-doped WO 3 nanorods structure, the Pd-400-Na/WO 3 NRs exhibit high sensing ability with ultra-high response to hydrogen (R a /R g = 218@25 ppm) and fast response time (3 s). The combination of experimental and theoretical results shows that Na doping effectively modulates the d-band center of Pd and enhances activation and desorption of H 2 on the Pd surface. The 1D porous structure also facilitates the diffusion of H 2 within the framework, and accelerate the charge transformation. Meanwhile, the surface Pd 0 sites are assigned as the surface active sites for H 2 adsorption and activation, and Pd 2+ sites facilitate the desorption process. Our work paves the new insights for the design of high performance H 2 sensing materials.

研究领域: 材料科学 · 化学工程 · 纳米技术
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Chemosensors · 2024 ·Vol. 12 ·期 3 ·43 · IF 3.7

Pd-Decorated ZnO Hexagonal Microdiscs for NH3 Sensor

Yi Li,Boyu Zhang,Juan Li,Zaihua Duan,Yajie Yang,Zhen Yuan,Yadong Jiang,Huiling Tai

The NH3sensor is of great significance in preventing NH3leakage and ensuring life safety. In this work, the Pd-decorated ZnO hexagonal microdiscs are synthesized using hydrothermal and annealing processes, and the gas sensor is fabricated based on Pd-decorated ZnO hexagonal microdiscs. The gas-sensing test results show that the Pd-ZnO gas sensor has a good response to NH3gas. Specifically, it has a good linear response within 0.5–50 ppm NH3at the optimal operating temperature of 230 °C. In addition, the Pd-ZnO gas sensor exhibits good repeatability, short response time (23.2 s) and good humidity resistance (10–90% relative humidity). This work provides a useful reference for developing an NH3sensor.

CAS / MDL: 5970-45-6 7647-10-1
研究领域: 材料科学 · 传感器技术 · 化学工程
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2021 · IF 19.503

Pd modified defective HNb3O8 with dual active sites for photocatalytic coproduction of hydrogen fuel and value-added chemicals

Xiaoli Li,Ting Wang,Ziqiang Zheng,Qing Yang,Can Li,Benxia Li

Developing photocatalysts for coproduction of hydrogen fuel and valuable chemicals is highly desired but still challenging. Herein, Pd-modified defective HNb 3 O 8 photocatalyst (denote as Pd/HNb 3 O 8 -H 2 ) consisting of dispersive Pd sites and abundant surface oxygen vacancies (V O s) was prepared via the thermal treatment of Pd 2+ -incorporated HNb 3 O 8 in H 2 /Ar gas. The existence of Pd favors the formation of V O s on HNb 3 O 8 , enabling the synchronous construction of Pd and V O dual active sites. The spectroscopy and photoelectrochemical studies demonstrate the advantages of Pd/HNb 3 O 8 -H 2 photocatalyst in promoting the separation and migration of photoinduced charge carries. The Pd/HNb 3 O 8 -H 2 photocatalyst exhibits the outstanding performance toward photocatalytic proton reduction coupled with selective benzyl-alcohol oxidation , achieving the optimal production rates of H 2 and benzaldehyde as high as 3.17 and 2.76 mmol·g cat −1 h −1 , respectively. The experimental and theoretical investigations have expounded the synergistic mechanism of Pd and V O dual active sites in boosting photocatalytic coproduction of H 2 and benzaldehyde.

研究领域: 材料科学 · 光催化化学 · 能源化学
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JOURNAL OF CATALYSIS · 2018 · IF 6.759

Hydrogen spillover enabled active Cu sites for methanol synthesis from CO2 hydrogenation over Pd doped CuZn catalysts

Bing Hu,Yazhi Yin,Guoliang Liu,Shengli Chen,Xinlin Hong,Shik Chi Edman Tsang

Surface modification with Pd is an effective way for improved activity in CO 2 hydrogenation to methanol over commercial Cu-ZnO catalysts via a so-called hydrogen spillover mechanism. However, there still lacks a quantitative analysis of hydrogen spillover effect and the nature of active sites after Pd modification remains unclear. In this work, we prepared a series of Pd-doped Cu-ZnO catalysts (Pd-CZ-x) with tunable Pd loading by using a facile polyol reduction method for a deep study of the promotion effect of Pd. With the increase of Pd/Cu molar ratio (x) from 0 to 0.04, there emerges a volcano-shaped relationship between methanol space time yield (STY) and Pd loading. 1% Pd doping can increase the methanol STY by 2.5 times and the methanol turnover frequency (TOF) by 3.5 times at 543 K, when compared to undoped Cu-ZnO. Kinetic studies show the activation energy required for methanol synthesis is greatly reduced from 59 kJ mol −1 over Cu-ZnO to 31 kJ mol −1 over Pd-CZ-0.01. Behind the volcano-shaped relationship is a balance between the hydrogen spillover effect of Pd and the reduced surface Cu area caused by Pd blocking. Chemisorption gives a quantitative analysis of an important type of activated Cu sites enabled by hydrogen spillover (Cu hs ). Importantly, it is found that the methanol STY correlates linearly with Cu hs surface area, suggesting that the activated Cu sites with the assistance of ZnO are real active sites for methanol synthesis from CO 2 hydrogenation.

CAS / MDL: 13820-53-6
研究领域: 催化化学 · 材料科学
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Catalysis Science & Technology · 2023 ·Vol. 13 ·期 6 ·1855-1865 · IF 5

Photocatalytic C–N coupling towards urea synthesis with a palladium-supported CeO2 catalyst

Shuyi Yang,Jiayi Deng,Jiaying Chen,Qingmei Tan,Tianren Liu,Ke Chen,Dongxue Han,Yingming Ma,Mengjiao Dai,Li Niu

The conversion of N2 and CO2 into urea through a photocatalytic C–N coupling reaction under ambient conditions serves as a novel green avenue for urea synthesis. However, the poor adsorption and C–N coupling capability of inert gas molecules hinder the efficient catalytic activity. Herein, palladium-decorated CeO2 (Pd–CeO2) was demonstrated as an efficient photocatalyst for C–N coupling reaction and delivered a remarkable urea yield rate of 9.2 μmol h−1 g−1, which was superior to that of pristine CeO2 (2.5 μmol h−1 g−1). Comprehensive investigations further endorsed that the emerged space-charge region in the CeO2(111)/Pd(111) interface not only effectively facilitates the targeted capture and activation of inert CO2 and N2 but also stabilizes the formation of key intermediates (*NCON). Besides, the effective inhibition of the endothermic *NNH intermediate is conducive to the subsequent C–N coupling process and the improvement of reaction selectivity. The reaction mechanism was studied in detail by density functional theory (DFT) with the formation of a C–N bond via a thermodynamically spontaneous reaction between *NN* and CO. This work provides novel insights into the conversion of CO2 and N2 into urea.

CAS / MDL: 7803-57-8
研究领域: 化学工程 · 材料科学 · 环境科学
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JOURNAL OF HAZARDOUS MATERIALS · 2013 · IF 3.925

Effect of silver or copper middle layer on the performance of palladium modified nickel foam electrodes in the 2-chlorobiphenyl dechlorination

Zhiqiao He,Junjun Sun,Jie Wei,Qiong Wang,Chengxiang Huang,Jianmeng Chen,Shuang Song

To enhance the activity of chemi-deposited palladium/nickel foam (Pd/Ni) electrodes used for an electrochemical dechlorination process, silver or copper was deposited electrochemically onto the nickel foam substrate (to give Ag/Ni or Cu/Ni) before the chemical deposition of palladium. The physicochemical properties of the resulting materials (Pd/Ni, Pd/Ag/Ni and Pd/Cu/Ni) were characterized by X-ray diffraction (XRD) and scanning electron microscopy (SEM), and their electrochemical catalytic activities were evaluated by monitoring the electrochemical dechlorination of 2-chlorobiphenyl (2-CB) in strongly alkaline methanol/water solution. The results show that the Pd/Ag/Ni and Pd/Cu/Ni electrodes had consistently higher electrocatalytic activities and current efficiencies (CEs) compared with the untreated Pd/Ni electrode. The Pd/Ag/Ni electrode exhibited the highest activity. The dechlorination was also studied as a function of Pd loading, the Ag or Cu interlayer loadings, and the current density. The Pd loading and the interlayer loadings both had positive effects on the dechlorination reaction. Increasing the current density increased the reaction rate but reduced the CE. The improvement of the electrocatalytic activities of the Pd/Ni electrode by applying the interlayer of Ag or Cu resulted from the enlargement of the effective surface area of the electrode and the adjustment of the metal H bond energy to the appropriate value, as well as the effective adsorption of 2-CB on Ag. Moreover, the high catalytic activity of the Pd/Ag/Ni electrode was maintained after six successive cyclic experiments, whereas Pd/Cu/Ni electrodes deactivate severely under the same conditions.

研究领域: 环境科学 · 电化学
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IONICS · 2017 ·Vol. 23 ·期 7 ·1861-1869 · IF 2.062

Preparation of carbon-supported Pd-decorated PtCu nanoparticles towards formic acid oxidation reaction

Suo Yange,Rong Chenbin,Guo Yuxin,Zhang Zhiguo,Hu Guilin,Xu Yousheng,Zhou Xinfa

This work reports the synthesis of a novel carbon-supported Pd-decorated PtCu nanocatalyst for formic acid oxidation. Without using surfactants or polymers, PtCu alloy was firstly prepared through simply co-reduction of Pt and Cu ions using ethylene glycol and sodium citrate as the reducing and stabilizing reagents. Then, Pd was decorated on the surface of PtCu through spontaneous replacement of Cu by Pd. XRD results suggest that the lattice parameters of the PtCu and Pd-decorated PtCu nanoparticles are smaller than that of Pt. TEM images show that all metallic nanoparticles are well dispersed on the carbon surface. The average particle size of the Pd-decorated PtCu nanoparticles is 2.9 nm. Electrochemical analysis suggests that the carbon-supported Pd-decorated PtCu nanocatalyst exhibits an enhanced activity for formic acid oxidation in comparison with the carbon-supported Pt and carbon-supported PtCu, as well as a high stability in acidic medium.

研究领域: 材料科学 · 电化学
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ELECTROCHIMICA ACTA · 2017 · IF 4.798

Preparation and Characterization of a Pd modified Ti/SnO2-Sb anode and its electrochemical degradation of Ni-EDTA

Lianghao Li,Zhuangpeng Huang,Xiaoxiao Fan,Zhen Zhang,Rongni Dou,Shulong Wen,Yuan Chen,Yuancai Chen,Yongyou Hu

An optimized metal oxide electrode (Ti/SnO 2 -Sb-Pd) was prepared via thermal decomposition and used in the electrochemical degradation of Ni-EDTA. The electrode was characterized by SEM, XRD, XPS, and electrochemical characterizations including linear-sweep voltammetry (LSV), cyclic voltammetry (CV) and chronopotentiometry (CP) techniques. It was found that Pd doping could effectively change the surface morphology and lattice parameters of the metal oxide electrode. Pd can facilitate the entry of more Sb into SnO 2 crystals and promote the reduction of Sb from the +5 to the +3 state. The interaction of these metals raised the oxygen evolution potential (OEP) and electrochemical surface area of the electrode, in addition to reducing the degradation potential and increasing the degradation current of Ni-EDTA. When the molar ratio of Pd:Sn was 2.5%, the electrode could simultaneously degrade 87.5% of Ni-EDTA and recycle 17.9% of elemental Ni on the cathode within 120   min. At the same time, with Pd doping, the lifetime of the electrode was increased more than 40 times, demonstrating good potential for application in industry.

研究领域: 材料科学 · 环境工程
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NEW JOURNAL OF CHEMISTRY · 2015 ·Vol. 39 ·期 6 ·4519-4525 · IF 3.086

Catalysis of the hydro-dechlorination of 4-chlorophenol by Pd(0)-modified MCM-48 mesoporous microspheres with an ultra-high surface area

Yansheng Liu,Xinlin Li,Xuanduong Le,Wei Zhang,Hao Gu,Ruiwen Xue,Jiantai Ma

MCM-48 mesoporous microspheres (M48N) with a pore size of 3.77 nm, an ultra-high surface area of 1250.77 m2 g−1 and a super-large pore volume of 1.52 cm3 g−1 were synthesized. The M48N microspheres were then modified with Pd, Pt and Ru nanoparticles using an incipient wetness impregnation technique. The modified M48N microspheres were investigated to determine their catalytic effect in the aqueous phase hydro-dechlorination (HDC) of 4-chlorophenol. The Pd–M48N, Pt–M48N and Ru–M48N catalysts were characterized by transmission electron microscopy, X-ray diffraction, nitrogen adsorption–desorption and X-ray photoelectron spectroscopy. The HDC experiments were performed using the fairly mild conditions of room temperature and an atmospheric pressure of H2. Pd–M48N showed a higher catalytic performance than Pt–M48N and Ru–M48N and various other Pd-based catalysts. The high catalytic performance of Pd–M48N resulted from the ultra-high surface area, super-large pore volume and unique pore structure of the M48N, which improved the mass transfer and increased the rate of adsorption–desorption of the compounds. This method has potential applications in the treatment of industrial wastewaters contaminated with chlorinated organic compounds.

研究领域: 环境科学 · 催化化学
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Journal of Environmental Chemical Engineering · 2024 · IF 7.4

Degradation mechanism and ecotoxicity analysis of levofloxacin by palladium-modified nano zero-valent iron doped coconut shell biochar

Yuxuan Tian,Shicong Luo,Edwin Hena Dawolo,Bingfa Chen,Ning Ding,Hong Liu

The palladium-modified nano zero-valent iron (nZVI) doped coconut shell biochar (Pd-nZVI/BC) was successfully obtained through bimetallic modification and liquid-phase reduction. The synthesized Pd-nZVI/BC was further enhanced by the addition of an H 2 O 2 co-catalyst for the removal of antibiotic levofloxacin (LVF). Results demonstrated that removal of LVF by Pd-nZVI/BC accomplished 94.6 % under proper conditions. Adsorption and degradation processes were involved in the LVF removal, and the predominant free radicals were •OH and •O 2- . Adsorption relied mainly on electrostatic interactions, π-π interactions, and hydrogen bonding. While demethylation, deamidation, quinolone ring aldolization, depiperazinylation, deacetylation, decarboxylation, dehydroxylation, and oxidative breakage of the piperazine ring occurred during the degradation processes. Based on the degradation pathways, the ecotoxicity of LVF and its degradation intermediates were compared and assessed. Results implied that majority of the antibiotic LVF pollutant was eliminated or mineralized, and the toxicity potential of LVF was reduced in the Pd-nZVI/BC system. Simultaneous biochar utilization and pollutants removal could be achieved.

研究领域: 环境科学 · 材料科学
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