JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2021
·
IF 4.464
Zhiyuan Lin,Wei Su,Song Zhang,Mingtao Zhang,Kexun Li,Jia Liu
A kind of Co 2 P embedded in nitrogen-doped carbon nanoframework (Co 2 PNC-NF) synthesized from directly carbonized Co-based metal-organic framework (ZIF-67) combined with phosphorus was utilized in the microbial fuel cell (MFC) to modify the active carbon air-cathode for the first time. Various techniques involving XRD, FESEM, TEM/EDS, BET and XPS were used to characterize the microstructure, morphology and surface chemical composition belonging to as-synthesized Co 2 PNC-NF. The electrochemical measurements revealed that the active carbon cathode modified by Co 2 PNC-NF got reduced resistance and optimized catalytic behavior in oxygen reduction reaction (ORR) process. The optimized MFC had a high maximum power density reaching 2001 mW m −2 , increasing by 123% compared with the bare active carbon cathode MFC. This result showed that combination between transition-metals phosphide and heteroatom-doped carbon matrices was beneficial to the improvement of MFC performance. Moreover, density functional theory calculations indicated that the special structure of double Co site of 001 face of Co 2 P can accelerate the ORR by boosting the cracking of OOH* group. Therefore, the Co 2 PNC-NF could be applied as an economical and efficient electrocatalyst in MFC to replace noble metal catalyst.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Lin Zhong,Hu Zhou,Ruifeng Li,Hao Cheng,Sheng Wang,Boyuan Chen,Yongyue Zhuang,Junfeng Chen,Aihua Yuan
Developing highly efficient oxygen electrocatalysts is of vital importance for rechargeable Zn-air batteries (ZABs). Herein, Co/CoO x nano-heterojunctions encapsulated into nitrogen-doped carbon sheets (NCS@Co/CoO x ) are fabricated via a dual-template-guided approach by using zeolitic imidazolate frameworks (ZIFs) as templates. The synergistic integration of structural and compositional advantages endows such catalyst with superior catalytic properties to benchmark noble-metal catalysts. To be specific, the hierarchical micro/mesopores affords massive mass transport channels and maximizes the exposure of accessible active sites, whereas the NCS matrix accelerates electron transfer and prevents the self-aggregation of active species during the electrocatalytic reaction. Moreover, abundant and synergistic Co-based active sites (CoO, Co 3 O 4 , Co-N x ) greatly promote the catalytic activity. As the cathode of both liquid and flexible solid-state ZABs, excellent device properties are achieved, outperforming those assembled with commercial Pt/C+RuO 2 catalyst. This work presents a feasible and cost-effective strategy for developing oxygen electrocatalysts derived from ZIFs templates.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Shaoda Huang,Shuanglong Lu,Hongyin Hu,Fangping Xu,Huining Li,Fang Duan,Han Zhu,Hongwei Gu,Mingliang Du
Although attentions have been devoted to developing Pd-based bimetallic nanocrystals towards the electrocatalytic oxygen reduction reaction (ORR) and ethanol oxidation reaction (EOR), the engineering of efficient bifunctional electrocatalysts with high atomic utilization still faces big challenges. Herein, we reported a facile one-pot template-free route to fabricate three-dimension hyper-dendritic PdZn nanocrystals (HD-PdZn NCs) that regulated by gas mixtures of carbon monoxide and hydrogen. The developed catalysts acted as robust bifunctional electrocatalysts for cathodic ORR and anodic EOR. Specifically, the engineered HD-PdZn NCs not only displayed superior mass activity (MA, 0.461 A mg Pd -1 ) and specific activity (SA, 0.393 mA cm −2 ) at 0.9 V, which were 5.2 and 5.0 times of commercial Pt/C, respectively, but also showed enhanced stability with only 3% loss of MA after 10,000 cycles for ORR. Density functional theory (DFT) calculations revealed the Zn implantation could facilitate the reduction of OOH* to OH* on the surface of Pd during the ORR process. Moreover, HD-PdZn NCs exhibited the highest EOR mass activity with a value of 3.45 A mg Pd −1 among benchmarked catalysts in alkaline solution. The advantageous structural features and electron effects are proposed to be responsible for the remarkable bifunctional activities. This work illustrates a facile method to fabricate highly efficient bifunctional electrocatalyst for energy conversation application.
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ACS Omega
·
2021
·
IF 3.512
Zhou Yang,Runmiao Yang,Guanxiu Dong,Meng Xiang,Jia Hui,Junfei Ou,Hengfei Qin
Water splitting is the most potential method to produce hydrogen energy, however, the conventional electrocatalysts encounter the hindrances of high overpotential and low hydrogen production efficiency. Herein, we report a carbon-based nanocomposite (denoted as CCW-x, x stands for the calcination temperature) derived from watermelon peels and CoCl2, and the as-synthesized CCW-x is used as the electrocatalyst. The overpotential and the Tafel slope of CCW-700 for oxygen evolution reaction (OER) is 237 mV at 10 mA cm–2 and 69.8 mV dec–1, respectively, both of which are lower than those of commercial RuO2. For hydrogen evolution reaction (HER), the overpotential of CCW-700 (111 mV) is higher than that of the widely studied Pt/C (73 mV) but still lower than those of lots of carbon-based nanomaterials (122–177 mV). In the light of CCW-700 is highly active for both OER and HER, we assembled a water-splitting electrocatalyst by employing nickel foam loaded with CCW-700 as the anode and cathode in 1 M KOH. The water-splitting voltage is only 1.54 V for the CCW-700//CCW-700 electrodes and 1.62 V for the RuO2//Pt/C ones. Therefore, the so-denoted CCW-x powder possesses good electrocatalytic hydrogen production efficiency.
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ELECTROCHIMICA ACTA
·
2020
·
IF 6.215
Denian Li,Huibing Chen,Yuyuan Zhang,Jizhang Yang,Haoran Yuan,Yong Chen
With quite limited use, biomass tar has been a long-standing issue that strongly impaired the cost-efficiency of biomass gasification. Here, a facile activation-annealing route for upcycling biomass tar into graphene nanohybrids with developed porosity and enriched pyridinic nitrogen was reported, whilst the metal-free product revealed with superior catalytic activities to the benchmark Pt/C and RuO 2 catalysts toward oxygen reduction reaction (ORR) and evolution reaction (OER). By associating the dual functionalities with products’ physiochemical properties, it was unveiled that those pyridinic-N and defects were accounted for the promoted oxygen reduction and evolution, respectively. Together with reinforced electric conductivity and hierarchical porosity and enlarged interface via ammonia annealing, the heterogeneously structured carbon catalyst finally endowed an assembled primary Zn-air battery with maximum energy density of 121 mW/cm −2 , in addition to robust stability against long-term running. This work highlights the great potential of biomass tar for advanced carbon materials , and therefore a novel strategy to address the tar-related challenges faced by gasification technologies.
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NEW JOURNAL OF CHEMISTRY
·
2020
·Vol. 44
·期 35
·14970-14978
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IF 3.288
Jingchuang Zhao,Yingzhen Zhang,Xianyu Kang,Yancai Li
Direct methanol fuel cells (DMFCs) have been extensively studied for developing a new non-precious metal catalyst to replace commercial platinum catalysts, due to their expensive cost and susceptibility to CO poisoning. In this work, nanocomposites of nickel oxide/nickel supported by N-doped carbon (NiO/Ni–N/C) were prepared by using a hydrothermal method and further carbonization at different temperatures. The surface morphology and composition of the NiO/Ni–N/C nanocomposites were characterized by using X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS). As observed through electrochemical experiments, the NiO/Ni–N/C nanocomposite modified glassy carbon electrode (NiO/Ni–N/C/GCE) exhibits high electrocatalytic activity for the methanol oxidation reaction (MOR) in alkaline solution. Among the nanocomposites, NiO/Ni–N/C carbonized at 500 °C (NiO/Ni–N/C500) displays the highest mass activity (1043 mA mgNi−1) at 0.73 V (vs. Ag/AgCl), which is much higher than that of Ni(OH)2/N–C and NiO/Ni–N/C carbonized at other temperatures (400, 600, and 700 °C). In addition, the catalytic activity of NiO/Ni–N/C500 is 2.12 times that of the commercial Pt/C. NiO/Ni–N/C500/GCE also possesses fast kinetics, excellent stability and CO tolerance. Therefore, the NiO/Ni–N/C500 nanocomposites have great application potential as MOR catalysts.
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ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Xiaoling Sun,Qiaojuan Gong,Yunxia Liang,Mingjie Wu,Nengneng Xu,Pengni Gong,Shuhui Sun,Jinli Qiao
Rational synthesis of bifunctional electrocatalysts with high performance and strong durability is highly demanded rechargeable metal–air battery. In this work, ZIF-derived Co9S8/C coated with conductive graphene nanosheet (Co9S8/GN) was synthesized by a simple solvothermal method and formed a stable double-carbon structure. As expected, the prepared Co9S8/GN catalyst exhibits a high catalytic activity (ΔE: 0.88 V) and long-term durability toward both oxygen reduction reaction and oxygen evolution reaction (ORR and OER), which is even superior to the Pt/C + Ir/C mixture (0.91 V). In addition, the Zn–air battery with the Co9S8/GN catalyst showed higher power density (186 mW cm–2) and more stable charge–discharge cycling performances (2000 cycles) than the Pt/C + Ir/C (118 mW cm–2). Based on these analysis results, the favorable catalytic performance of ORR/OER should be illustrated by the following reasons: (i) large specific surface area and unique mesoporous structure, providing abundant active sites; (ii) good conductivity, accelerating the electrons transfer; and (iii) the unique stable “double-carbon” structures (metal–S–C–C), preventing the agglomeration of metal sulfide, building new quick transfer pathway, and forming the strong electron coupling ability and synergistic effect.
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Tungsten
·
2020
·Vol. 2
·期 2
·194-202
·
IF 0
Yu Xue-Ping,Yang Chan,Song Pin,Peng Juan
Ultra-small MoS 2 quantum dots (QDs) with an average size of 2.48 nm coated on Au nanoparticles with a core-satellite structure (Au/MoS 2 QDs) are successfully prepared by a self-assembly strategy through the strong bonding between Au and S. Benefited from the unique structure, the Au/MoS 2 QDs hybrid exhibits outstanding electrocatalytic performance toward hydrogen evolution reaction (HER). The Au/MoS 2 QDs hybrid needs overpotentials of 112, 146, and 206 mV to approach current densities of 10, 20, and 50 mA·cm −2 in 0.5 mol·L −1 H 2 SO 4 (pH = 0.3), respectively. And a low Tafel slope (83 mV·dec −1 ) is obtained. The catalyst also displays satisfactory stability and durability, indicating a negligible current density loss after 20 h of electrolysis. The high hydrogen generation activities and stability are attributed to the great number of active sites, high conductivity and synergistic effects between gold nanoparticles (Au NPs) and MoS 2 QDs. Last but not least, this strategy opens up a favorable way to combine MoS 2 QDs with other metals.
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NEW JOURNAL OF CHEMISTRY
·
2020
·Vol. 44
·期 40
·17313-17322
·
IF 3.288
Guigui Liu,Chao Shuai,Zunli Mo,Ruibin Guo,Nijuan Liu,Xiaohui Niu,Qibing Dong,Jia Wang,Qinqin Gao,Ying Chen,Wentong Liu
The design and preparation of highly efficient and durable non-noble metal electrocatalysts for overall water splitting is pivotal for actualizing large-scale water splitting via electrolysis. Herein, porous Ni0.85Se nanospheres anchored on reduced graphene oxide (RGO) (Ni0.85Se/RGO) were synthesized via a one-step hydrothermal method. Following explorations of the hydrothermal temperature and reaction time, the optimized Ni0.85Se/RGO exhibited extraordinary oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) performance in 1.0 M KOH solution, providing an overpotential as small as 320 mV at a current density of 30 mA cm−2 and a low Tafel slope of 91 mV dec−1 for the OER, and an overpotential of 169 mV at a current density of 10 mA cm−2 and a low Tafel slope of 65 mV dec−1 for the HER. A current density of 10 mA cm−2 at 1.64 V and high stability can be obtained upon using Ni0.85Se/RGO as both the cathode and anode for overall water splitting under alkaline conditions; this was attributed to the merits of both the porous structure of Ni0.85Se and the high conductivity of RGO. This work provides a meaningful exploration of the synthesis of 3d-transition-metal-chalcogenide- and carbon-based composite electrocatalysts via a hydrothermal reaction for water splitting, and provides a general method.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2020
·
IF 4.65
Sishun Wang,Kejun Bu,Dong Wang,Chong Zheng,Xiangli Che,Zhen Han,Fuqiang Huang
A new platinum-based ternary selenide, Pt 3 Pb 2 Se 2 was successfully synthesized at 1123 K by using a traditional solid-state method. It crystallizes in a orthorhombic structure with the Cmcm space group, and consists of quasi-2D [Pt 3 Pb 2 Se 2 ] layers connected by inherent Pt–Pb bonds. It is related to the parkerite structures with half transition metal occupation. Therefore, it belongs to the half anti-perovskite family structure. The R-T curve reveals its metallic behavior and shows high conductivity (RRR = 20.5) at room temperature. The X-ray photoelectron and ultraviolet photoelectron spectroscopy spectrums were collected. It has low work function ( ϕ = −4.02 eV). First principles calculations were consistent with the experimental results.
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Nanoscale
·
2021
·Vol. 13
·期 4
·2632-2638
·
IF 7.79
Xiaowei Chen,Wei Wang,Xuejiao Chen,Xinyan Liao,Zixi Lyu,Kai Liu,Shuifen Xie
Platinum (Pt)-based nanocatalysts with a high density of surface atomic steps hold great prospects in electrocatalysis. However, the structural instability under harsh redox conditions is still a rigorous challenge. Here, we demonstrate that ternary PtCoRh alloyed spiral nanowires (SNWs), which have the advantages of one-dimensional nanowires, alloy synergy, surface atomic steps, and anti-corrosive Rh incorporation, can serve as active and robust MOR electrocatalysts in acidic media. The results showed that the Pt77Co11Rh12 SNWs delivered the highest mass activity (1.48 A mg−1) and specific activity (4.76 mA cm−2), as well as the best durability in the long-term MOR test, compared with the Pt85Co10Rh5 and Pt85Co15 SNWs and Pt black. Further inspections of the morphology, composition, and electronic structure revealed that the incorporated Rh atoms not only stabilized the highly rugged SNWs and the easily leaching Co atoms but also delicately tuned the electron transfer among the three metallic elements, leading to the enhancement of MOR activity, structural stability and anti-CO-poisoning ability. Our work provides a rational strategy for the development of highly efficient and durable alcohol oxidation electrocatalysts.
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Sustainable Energy & Fuels
·
2020
·Vol. 5
·期 2
·556-563
·
IF 5.503
Fengan Han,Jingyuan Xu,Guangyi Li,Jilei Xu,Aiqin Wang,Yu Cong,Tao Zhang,Ning Li
Aviation fuel range high-density bicycloalkanes were selectively synthesized with methyl isobutyl ketone (MIBK) and aromatic aldehydes which can be derived from lignocellulose. First, a series of aviation fuel precursors were obtained by the solvent-free aldol condensation of methyl isobutyl ketone (MIBK) and aromatic aldehydes. Among the investigated catalysts, Amberlyst-15 resin exhibited the highest activity. On the basis of characterization, the good performance of Amberlyst-15 resin can be attributed to its bigger surface area, and higher acid site amount and acid strength. Subsequently, the aldol condensation products were further converted to bicycloalkanes by solvent-free hydrodeoxygenation (HDO). A commercial Ru/C catalyst exhibited the highest activity for the HDO process. Over it, high yields (∼95%) of aviation fuel range bicycloalkanes were achieved under mild conditions. According to characterization results, the excellent performance of the Ru/C catalyst might be rationalized by its relatively higher acid strength and better metal dispersion. The bicycloalkanes obtained in this work have high densities (0.895–0.902 g mL−1) and low freezing points (223.2–230.0 K). In real applications, they can be used as high-density aviation fuels or additives to improve the volumetric heat values and thermal stability of current aviation fuels.
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