Nano Research
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2017
·Vol. 10
·期 7
·2482-2494
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IF 7.354
Cui Shiqiang,Li Li,Ding Yaping,Zhang Jiangjiang,Wu Qingsheng,Hu Zongqian
Uniform, ordered mesoporous ZnCo 2 O 4 (meso-ZnCo 2 O 4 ) nanospheres were successfully synthesized using a sacrificing template method. The meso-ZnCo 2 O 4 nanospheres were used for the first time for H 2 O 2 biosensing and in glucose biofuel cells (GBFCs) as an enzyme mimic. The meso-ZnCo 2 O 4 nanospheres not only exhibited excellent catalytic performance in the H 2 O 2 sensor, achieving a high sensitivity (658.92 μA·mM –1 ·cm –2 ) and low detection limit (0.3 nM at signal-to-noise ratio (S/N) = 3), but also performed as an excellent cathode material in GBFCs, resulting in an open circuit voltage of 0.83 V, maximum power density of 0.32 mW·cm –2 , and limiting current density of 1.32 mA·cm –2 . The preeminent catalytic abilities to H 2 O 2 and glucose may be associated with the large specific surface area of the mesoporous structure in addition to the intrinsic catalytic activity of ZnCo 2 O 4 . These significant findings provide a successful basis for developing methods for the supersensitive detection of H 2 O 2 and enriching catalytic materials for biofuel cells.
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CHEMISTRY-A EUROPEAN JOURNAL
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2017
·Vol. 23
·期 32
·7791-7797
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IF 5.317
Sanjeevi Jayakumar,Arindam Modak,Miao Guo,He Li,Xiangping Hu,Qihua Yang
Graphical Stability from supports : Ultrasmall platinum nanoparticles (Pt NPs) stabilized by triphenylphosphine-modified Pt/SiO 2 show high activity and good selectivity in acetophenone and phenylacetylene hydrogenation reactions compared with those on bare Pt/SiO 2 because of strong metal–support interactions (see figure). Chemoselective hydrogenation of substrates with more than one functional group that could be hydrogenated is quite challenging and is of fundamental importance. Here, the enhanced chemoselectivity of ultrasmall (<1 nm) platinum nanoparticles (NPs) stabilized on silica modified with triphenylphosphine (PSiO 2 ) in hydrogenation reactions is reported. Platinum NPs on PSiO 2 exhibit much higher selectivity than those on SiO 2 in the hydrogenation of acetophenone to 1-phenylethanol (99.9 versus 36 %) and hydrogenation of phenylacetylene to styrene (85 versus 52 %). The results of NMR spectroscopy, X-ray photoelectron spectroscopy, and in situ CO adsorption FTIR spectroscopy indicate the existence of strong interactions between triphenylphosphine and Pt NPs. Consequently, Pt NPs on PSiO 2 have smaller particle sizes and more positive Pt 4 f binding energy than those of Pt/SiO 2 ; these are the main contributors to the superior chemoselectivity of Pt NPs. The organically modified silica could act as an efficient solid ligand for tuning the catalytic performance of metal NPs.
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ELECTROCHEMISTRY COMMUNICATIONS
·
2017
·
IF 4.396
Fengjin Qu,Xiaoyan Ma,Lin Zhu,Fang Chen
A new photoswitchable electrode triggered by a brief light signal was fabricated by depositing an azobenzene-containing copolymer on an indium tin oxide substrate decorated with gold nanoparticles . The polymer formed a compact, complete thin film on the electrode surface using the Langmuir–Schaefer technique and offered reversible and stable switching performance. The conductivity and hydrophilicity of the electrode changed under UV/visible light due to the photoisomerization of the azobenzene moieties in the polymer film, influencing electron transfer and mass transport at the electrode. The electrochemical characterization demonstrated that the electrode exhibited reversibly switchable electrochemical behavior. In its active state, the as-prepared electrode possessed efficient electrocatalytic capability towards uric acid oxidation with a maximum anodic current density of 0.97 mA·cm − 2 . The uric acid/air fuel cell assembled from the photo-triggered anode and a Pt/C-modified cathode operated with an open circuit voltage of 0.12 V and a maximum power density of 41.33 μW·cm − 2 . The cell exhibited reversible switching performance (four cycles) and high stability: after one month the power output was 94.2% of the original maximum value.
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CHINESE JOURNAL OF CATALYSIS
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2016
·
IF 2.628
Tingting Zhang,Chuansheng He,Linbo Li,Yuqing Lin
The oxygen reduction reaction (ORR) is traditionally performed using noble-metals catalysts, e.g. Pt. However, these metal-based catalysts have the drawbacks of high costs, low selectivity, poor stabilities, and detrimental environmental effects. Here, we describe metal-free nitrogen-doped carbon nanoblocks (NCNBs) with high nitrogen contents (4.11%), which have good electrocatalytic properties for ORRs. This material was fabricated using a scalable, one-step process involving the pyrolysis of tris(hydroxymethyl)aminomethane (Tris) at 800 °C. Rotating ring disk electrode measurements show that the NCNBs give a high electrocatalytic performance and have good stability in ORRs. The onset potential of the catalyst for the ORR is −0.05 V (vs Ag/AgCl), the ORR reduction peak potential is −0.20 V (vs Ag/AgCl), and the electron transfer number is 3.4. The NCNBs showed pronounced electrocatalytic activity, improved long-term stability, and better tolerance of the methanol crossover effect compared with a commercial 20 wt% Pt/C catalyst. The composition and structure of, and nitrogen species in, the NCNBs were investigated using Fourier-transform infrared spectroscopy, scanning electron microscopy, X-ray photoelectron spectroscopy, and X-ray diffraction. The pyrolysis of Tris at high temperature increases the number of active nitrogen sites, especially pyridinic nitrogen, which creates a net positive charge on adjacent carbon atoms, and the high positive charge promotes oxygen adsorption and reduction. The results show that NCNBs prepared by pyrolysis of Tris as nitrogen and carbon sources are a promising ORR catalyst for fuel cells.
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ACS Catalysis
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2016
·
IF 9.307
Zhongzhe Wei,Yiqing Chen,Jing Wang,Diefeng Su,Minghui Tang,Shanjun Mao,Yong Wang
Porous nitrogen-doped graphene layers encapsulating cobalt nanoparticles (NPs) were prepared by the direct pyrolysis process. The resulting hybrids catalyze the hydrogenation of diverse quinoline compounds to access the corresponding tetrahydro derivatives (THQs), important molecules present in fine and bulk chemicals. Near-quantitative yields of the corresponding THQs were obtained under optimized conditions. Notably, various useful substituted quinolines and other biologically important N-heteroarenes are also viable. The enhanced stability of the catalyst is ascribed to the encapsulation structure, which can enormously reduce the extent of leaching of base metals and protect metal NPs from growing larger. The achieved success in the encapsulation of metal NPs within graphene layers opens an avenue for the design of highly active and reusable heterogeneous catalysts for more challenging molecules.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Fanjia Sun,Jianbing Zang,Zhiwei Hou,Xueqing Tian,Rui Zhu,Youbin Zheng,Yanhui Wang,Liang Dong
The design of low-cost, highly active, and stable electrocatalysts is pivotal for advancing water electrolysis technologies. In this study, carbonyl iron powder (CIP) was anchored within the pores of nickel foam (NF) by electroplating nickel, creating nickel iron foam-like (NFF-L) substrates. Subsequently, nickel–iron hydroxide (NiFe-OH) was synthesized on the NFF-L substrate employing an autogenous growth strategy, followed by a phosphating treatment that produced a nanoflower-like NiFe bimetallic phosphide heterostructure catalyst (Fe 2 P-Ni 2 P@NFF-L). This novel method of substrate filling enhanced space utilization, while the presence of micropores and mesopores on the nanosheet surfaces facilitated electrolyte infiltration and ion diffusion, thereby significantly increasing the specific surface area. The formation of a two-phase heterointerface accelerated electron transmission and transfer, enhancing water dissociation and the adsorption of hydrogen adatoms (H ad ). In addition, under anodic oxidation conditions, the dynamic surface reconstruction facilitated a synergistic interaction between the highly active β-NiOOH and α-FeOOH phases, which significantly contributed to the catalyst’s exceptional intrinsic activity for the oxygen evolution reaction (OER).
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International Journal of Electrochemical Science
·
2024
·
IF 1.3
Baikai Zhang,Xiaohui Li,Maochang Liu
An important area of research is the creation of non-precious metal catalysts with increased catalytic activity and stability for the electrolysis of water to produce hydrogen. A viable and effective method for altering the surface structure of electrocatalysts and improving their performance is morphology control. In this study, the amount of ammonium fluoride (NH 4 F) used in the hydrothermal process was changed to create a range of nickel sulfide (NiS) electrocatalysts with tunable morphologies. The improved NiS catalyst demonstrated exceptional performance in the hydrogen evolution process (HER) because of its expansive active area, elevated surface activity, and gas diffusion channels. In particular, it showed a low Tafel slope of 65.90 mV dec −1 in 1 M KOH electrolyte solution and an overpotential of 97 mV at a current density of 10 mA cm −2 . Remarkably, the NiS electrocatalyst maintained its excellent HER performance even after 60-hour durability test. These findings underscore the significance and feasibility of morphology control in achieving desirable catalytic activity.
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IONICS
·
2024
·
IF 2.4
Duan Jinrong,Si Fang,Wang Jiafen,Lu Linlin,Liu Jia,Song Yanyan,Mo Jiahui,Yu Jincui,Gao Jinlong
Fuel cell is considered the best candidate power source because of its high energy conversion rate, large capacity, and zero emission. However, noble metal catalysts as a key core material have some problems, such as high cost and poor durability. Therefore, in this paper, the active self-supporting nanoporous Pd–Ag catalysts are successfully formed by cryogenic treatment and one-step dealloying treatment of Al-Pd–Ag ribbons. The surface of the catalyst ligaments shows a certain degree of preferred orientation for high-index facets (220) and (311). The results show that the activity and stability of the catalysts for methanol electrocatalytic oxidation are significantly improved under the synergistic effect of special configuration and promoter Ag. The electrocatalytic activity of the catalysts is about 9.7 and 15.2 times that of commercial Pt/C and commercial Pd/C catalysts, respectively. After 5000 s, the current density of the 1800 rpm-deep2 sample is 382.88 mA·mg −1 , which is about 14.1 times and 39.9 times that of commercial Pt/C catalyst and commercial Pd/C catalyst.
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Journal of Materials Chemistry A
·
2024
·Vol. 12
·期 47
·33301-33313
·
IF 10.7
Yantong Long,Guoliang Zhao,Liuxin Yang,Yongjun Xu,Chen Xu
Efficient bifunctional catalysts for hydrogen/oxygen evolution reactions (HER/OER) are critical for industrial application of overall water splitting. Herein, a self-supported nanostructure consisting of CoNi–P and embedded carbon dots (denoted as CoNi–P/CDs/NF) with large specific surface area has been designed and fabricated, through a phosphorization process on precursors grown on 3D porous Ni foam. The resultant electrocatalyst exhibited excellent electrocatalytic performance for both the HER (45.2 mV@10 mA cm−2) and OER (184.8 mV@20 mA cm−2) under alkaline conditions. The cell voltage of the full water splitting device assembled was only 1.50 V to achieve 20 mA cm−2 and exhibited great durability benefiting from the self-supported nanostructure. The density functional theory (DFT) calculations and XPS analysis suggest that the synergistic coupling effect between CDs and substrate CoNi–P could tune the electronic structure. Moreover, the embedded CDs increase electrical conductivity and active sites of the catalyst. Both of these and the high specific surface benefited from the 1D/3D hierarchical structure could explain the excellent electrocatalytic performance. The rational materials design of 1D/3D hierarchical structured non-noble bimetallic phosphide catalysts in this work may suggest a new strategy for designing bifunctional electrocatalysts.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2025
·
IF 4.1
Zeyu Jin,Yuelin Wang,Linshan Zhu,Jingzi Zhang,Xi Lin
Oxygen evolution reaction (OER) plays an important role in the energy conversion industry. Despite the prevalent reliance on noble metals for their superior catalytic attributes, their high cost and limited availability present significant challenges. Reducing the use of noble metals in catalysts while maintaining catalytic activity and stability in various chemical environments is a major challenge in heterogeneous catalysis. In this study, we have strategically enhanced the catalytic performance of the Cr 2 O 3 oxide by introducing multiple transition metal dopants to modulate its electronic structure. It is found that doping Ni/Co/Cu/Ru into the Cr 2 O 3 oxide results in the best OER performance, which outperforms RuO 2 and other reported materials. We further improved the cycling stability of the multi-component catalyst by coating amorphous carbon on its surface. Specifically, with an OER overpotential of merely 210 mV at 10 mA cm −2 and a low Tafel slope of 59.5 mV dec −1 , the catalyst exhibits remarkable catalytic efficiency. More importantly, it can withstand high current tests exceeding 100 mA cm −2 for over 80 h without significant degradation of its OER catalytic performance. In addition, the catalyst exhibits exceptional hydrogen evolution reaction (HER) performance which is close to Pt/C, making it suitable for use as a bifunctional water splitting device. These findings have opened up a new field for the design and application of multi-component catalysts.
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Journal of Energy Storage
·
2024
·
IF 8.9
Heju Gao,Qihao Wu,Jiahui Jiang,Ting Zhao,Yuying Feng,Chunyan Wu,Guancheng Xu,Li Zhang
Reasonable construction of efficient bifunctional catalysts for the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER) counts a great deal for the development and application of rechargeable zinc-air batteries. Herein, we prepared nano-sized heterostructural particles of cobalt phosphides (CoP/Co 2 P) confined in N, P-codoped cubic through simple grinding combined with vapor deposition method using the Co formic-acid framework (Co-FF) as the precursor. Benefit from the synergistic effect between the coexistence of abundant active sites including Co sites derived the CoP/Co 2 P nanoparticles, graphitic-N, pyridinic-N species and regulation of heterojunction interface electrons, the CoP/Co 2 P@NPC-800 catalyst exhibited excellent bifunctional catalytic activity toward ORR and OER, slightly better than commercial 20 % Pt/C. The liquid zinc-air battery demonstrates a specific capacity of 720.1 mAh g −1 and outstanding stability exceeds 250 h, comparable to 20 % Pt/C. Moreover, the flexible zinc-air battery can maintain good stability under different angles of bending. This study has a certain theoretical guiding significance for the rational regulation of the phase of cobalt-based phosphide to fabricate bifunctional oxygen catalysts for metal-air battery applications.
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FUEL
·
2024
·
IF 6.7
Yang Liu,Shaokai Ma,Shiqing Zhang,Fang Liu,Ying Wang,Xinyu Sun,Ying Li,Yanming Xue,Chengchun Tang,Jun Zhang
Efficient and sustainable hydrogen production via water electrolysis relies on the utilization of highly active electrocatalysts for the oxygen evolution reaction (OER). Birnessite (δ-MnO 2 ), a type of manganese oxide with a local atomic structure similar to the oxygen-evolving complex in photosystem II, has emerged as a highly promising OER catalyst. Despite considerable efforts have been dedicated to enhancing its activity, the crucial aspect of stability has been often overlooked. Herein, Ti ions have been selectively incorporated into the in-layered lattice of δ-MnO 2 nanosheet arrays using a hydrothermal method, aiming to enhance the stability without reducing its activity. The resulting optimal Ti-MnO 2 catalyst demonstrates enhanced OER activity in alkaline electrolyte, exhibiting an impressive 85 mV reduction in overpotential at 10 mA cm −2 , surpassing the initial MnO 2 (495 mV reduced to 410 mV). Remarkably, it shows exceptional durability, with negligible performance decrease observed over the entire 50-hour testing period. It has been demonstrated that the incorporation of Ti serves a dual purpose: it adjusts the electronic structure around Mn, enhancing activity, and simultaneously stabilizes the Mn 3+ active sites, resulting in exceptional durability. Furthermore, density functional theory (DFT) calculations provide additional confirmation of the optimized electronic structure of MnO 2 achieved through Ti doping, leading to a reduction in the free energy of adsorbed intermediates and expediting the kinetics of the OER process. Our findings open a pathway for enhancing OER stability and activity by doping electrocatalytic inert ions into the lattice of MnO 2 , applicable not only to Mn-based oxides but also other non-precious metal-based electrocatalysts.
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