JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
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IF 9.965
Zhiqiang Zhang,Xiaofeng Lin,Shuli Tang,Haijiao Xie,Qitong Huang
Efficient, stable and low-cost catalysts are essential for improving the efficiency of hydrogen evolution reactions . Herein, the MoO 2 @Ni 2 P heterostructure electrocatalyst was synthesized in a self-supported system on a carbon paper (CP) by two-step deposition and phosphorization at low temperature. The self-supported nanoarray structure makes the catalyst to effectively and efficiently transfer electrons and exposes more of its active sites. Moreover, the strong interaction between Ni 2 P and MoO 2 helps to effectively optimize the electronic structure. The density of states calculations demonstrate that there is an increase in the density of electronic states near the MoO 2 /Ni 2 P Fermi level . This shows that MoO 2 /Ni 2 P has fast charge transfer kinetics. MoO 2 modulates the d-band center of nickel, resulting in moderate adsorption/desorption of hydrogen. The above results show that MoO 2 @Ni 2 P has good hydrogen evolution activity. The experimental results show that the overpotential (η 10 ) of MoO 2 @Ni 2 P/CP in the alkaline environment is only 57 mV with a Tafel slope of 61 mV dec −1 . It is similar to the commercial noble-metal catalysts and outperforms most reported catalysts.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2022
·
IF 6.371
Shi Chen,Wenjing Liang,Xinyi Wang,Yueqi Zhao,Shuo Wang,Zheng Li,Shengmei Wang,Li Hou,Yang Jiang,Faming Gao
Transition metal sulfides (TMSs) are widely used in energy storage and energy conversion systems because of their excellent electrochemical properties . However, their application is restricted by a low electron transfer efficiency, few active sites and poor stability. In this paper, CoNi bimetallic sulfides supported by carbon skeleton (CoNi-SP/NPC) were prepared using bimetallic organic frameworks (MOFs) as templates and modified with phosphorus doping. Compared with single metal sulfides, the bimetallic sulfides are more favorable for electron transfer in the catalytic process. Meanwhile, the carbon skeleton support gives the catalyst higher mechanical stability, and the P-doping brings more active sites into to contact with the aqueous solution. The overpotential of CoNi-SP/NPC catalyst is only 105 mV at 10 mA cm −2 for hydrogen evolution reaction (HER) and 313 mV at 100 mA cm −2 for oxygen evolution reaction (OER). In addition, CoNi-SP/NPC also displays remarkable performance in the course of overall water splitting, which can achieve 50 mA cm −2 at only 1.8 V and remains good stability for 12 h. This work proposes a feasible strategy to synthesize highly efficient water splitting electrocatalysts .
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Menglei Yuan,Lei Zhang,Tianxin Wang,Yiming Liu,Qiongguang Li,Jinxiong Wu,Junwu Chen,Jintong Zhang,Hailun Yang,Guangjin Zhang
Electrocatalytic water splitting in an alkaline medium is recognized as the promising technology to sustainably generate clean hydrogen energy via hydrogen evolution reaction (HER), while the sluggish water dissociation and subsequent *H adsorption steps greatly retarded the reaction kinetics and efficiency of the overall hydrogen evolution process. Whilst nitrogen (N)-doped carbon-based materials are attractive candidates for promoting HER activity, the facile fabrication and gaining a deeper insight into the electrocatalytic mechanism are still challenging. Herein, inspired by the Diels-Alder reaction, we precisely tailored six-membered pyridinic N and five-membered pyrrolic N sites at the edge of the carbon substrates. Comprehensive analysis validates that the participation of pyridinic N (electron-withdrawing) and pyrrolic N (electron-releasing) will induce the charge rearrangements, and further generate local electrophilic and nucleophilic domains in adjacent carbon rings, which guarantees the occurrence of water dissociation to generate protons and the subsequent adsorption of *H intermediates through electrostatic interactions, thereby facilitating the overall reaction kinetics. To this end, the optimal NC-ZnCl 2 -25 % electrocatalysts present excellent alkaline HER activity (η 10 = 45 mV, Tafel slop of 37.7 mV dec -1 ) superior to commercial Pt/C.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Qing-Qing Pang,Xue Bai,Xin Du,Shuo Zhang,Zhong-Yi Liu,Xin-Zheng Yue
Constructing highly active electrocatalysts towards hydrogen evolution reaction (HER) in both alkaline and acidic media is essential for achieving a sustainable energy economy. Here, a facile ethylene glycol reduction strategy was employed to design the nickel-ruthenium nanocrystals (Ni-Ru NC) with an exposed highly active Ru (1 0 1) facet as an efficient electrocatalyst for HER. Testings show Ni-Ru NC outperforms the benchmark catalyst Pt/C by delivering extraordinarily low overpotentials of 21.1 and 70.9 mV to drive 10 mA cm −2 in acidic and alkaline solutions, respectively. The results of experimental and theoretical studies suggest that Ni can modulate the electronic structure of the Ru NC and optimize the hydrogen adsorption free energy on Ru’s surface, which accelerates the charge transfer kinetics and enhances the HER performance. The study support the potential application of facet-modulated Ru-based HER eleccatalyst in an alkaline environment.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2023
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IF 7.2
Peng Cui,Tongheng Wang,Xuhai Zhang,Chongyang Ba,Yangkun Wu,Kai Peng,Yuqiao Zeng,Jianqing Jiang
Though various active electrocatalysts for hydrogen evolution reaction (HER) have been reported, it remains a challenge to develop efficient non-noble HER catalysts with pH-independent catalytic activity and high stability. In this work, novel porous NiCoCuP was prepared by combining the dynamic hydrogen bubble templated deposition with a low-temperature phosphorization process. The three-dimensional hierarchical porous structure provided the NiCoCuP with both self-supporting ability and ideal channels for fast mass transportation. As a consequence, the NiCoCuP foam exhibited excellent HER catalytic activity and outstanding durability over the entire pH range.
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NEW JOURNAL OF CHEMISTRY
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2022
·Vol. 46
·期 23
·11389-11397
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IF 3.925
Baoli Wang,Yuhao Huang,Yijing Ai,Yucen Yao,Fan Shi,Shiguan Xu,Zejun Zhang,Xianghui Wang,Wei Sun
Developing non-noble and high-performance electrocatalysts towards the hydrogen evolution reaction (HER) in both acidic and alkaline media remains a stern challenge. Herein, the composite of P-doped Mo2C and a hierarchically ultrathin N, P-doped carbon nanoribbon network (P-Mo2C/NPC) is proposed through a facile simultaneous phosphating-carbonization strategy, in which biomass and phosphomolybdic acid (PMA) were employed as the carbon precursor and metal precursor, respectively. The doping of the electronegative P heteroatom increases the active sites, weakens the Mo–H bond strength in the HER, and facilitates the electron transfer. Consequently, the synthesized catalyst exhibits good intrinsic activity towards the HER, and shows low overpotentials of 172 mV and 118 mV to afford the current density of 10 mA cm−2 in 0.5 M H2SO4 and 1.0 M KOH electrolyte, respectively. Furthermore, the synthesized catalyst can sustain 24 h with stable performance, which is greatly favorable for industrial applications. This work may shed some light on the rational design and manufacture of HER electrocatalysts with high compatibility to different electrolytic environments.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2022
·
IF 7.139
Lan Wang,Ning Gong,Zhou Zhou,Wenchao Peng,Yang Li,Fengbao Zhang,Xiaobin Fan
Developing highly efficient, durable and noble-metal-free electrocatalysts for hydrogen evolution reaction (HER) in a wide pH range is the key to achieve sustainable energy cycle. Modulating the electronic characteristics of catalysts is of great important to enhance their electrocatalytic performance. Herein, we successfully design a self-supported multi-element transition metal phosphide (V-CoP/Ni 2 P/NF) electrocatalyst by V-doping and interface engineering. According to DFT calculations, V dopants and the synergistic effect between CoP and Ni 2 P can bring optimal hydrogen/water adsorption free energies . Meanwhile, the 3D cross-linked network structure could expose abundant active sites and facilitate ions diffusion/electron transfer. As a result, the V-CoP/Ni 2 P/NF catalysts exhibit superior electrocatalytic activities with extremely low overpotentials of 20, 58 and 79 mV to deliver a current density of 10 mA cm −2 for HER in alkaline, neutral and acidic electrolytes, respectively. Moreover, they also display outstanding long-term stability. This electronic modulation strategy provides a promising pathway for energy-related catalysis processes.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2022
·
IF 7.139
Kun Qian,Fang Fang,Yifeng E,Yao Xu,Xiyuan Tong,Peng Chen,Lu Han,Zhuozhe Li
One of the important factors determining the expansion of the application domain of direct methanol fuel cell (DMFC) is its energy density . The bismuth-nickel doped LTA zeolite was as-synthesized in hydrothermal condition and applied into the electrochemistry catalysis of methanol oxidation reaction (MOR) with high performance in the methanol concentration ranging from 0.5 M to 35 M without observed catalyst poisoning . A trace amount of Bi and Ni atoms are highly dispersed on the opening window of the zeolitic surface by the electrochemical rearrangement process. The surface of the LTA structure zeolite is a good carrier for the metal cations with Na cations which could be replaced in hydrothermal crystalline process while the inner direct pores provide a channel for CO gas to escape and prevent catalyst poisoning in electrochemistry progress. Through the comparative study with the Bi doped LTA, Ni doped LTA and the commercial Pt/C catalyst, the Bi and Ni doped LTA reveals higher performance in monatomic catalytic efficiency and electrochemical stability. And through the mutual interaction of diatomic, the doped zeolite material highly improves the energy density of methanol fuel cells and reduces the cost of the cells concerning the absence of noble metals.
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ELECTROCHIMICA ACTA
·
2022
·
IF 7.336
Miaojing Pan,Wei Chen,Guangfu Qian,Tianqi Yu,Zhenglin Wang,Lin Luo,Shibin Yin
Exploiting highly efficient catalysts to treat wastewater containing urea via electrocatalytic oxidation is significant for environmental protection and energy requirements. Hence, a carbon-encapsulated Co 3 V decorated Co 2 VO 4 nanosheets catalyst (Co 3 V@C/Co 2 VO 4 ) is synthesized to accelerate urea oxidation reaction (UOR) and hydrogen evolution reaction (HER). It displays low potentials of 1.31 V and −51 mV to drive ±10 mA cm −2 in 1.0 M KOH + 0.5 M urea solution for UOR and HER, respectively. Impressively, for urea-assisted water splitting, only 1.37 V is needed to deliver 10 mA cm −2 , and it can maintain at 100 mA cm −2 for 100 h without significant activity decay. The good performance is attributed to the heterojunction between alloy and metal oxide, as well as the carbon-encapsulating and distinctive nanosheets structure. This study provides a novel choice for developing low cost and high-performance bifunctional catalysts to deal with urea-contained wastewater and produce hydrogen.
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CHEMOSPHERE
·
2022
·
IF 8.943
Chengzhi Wang,Guanlan Wu,Xiaolin Zhu,Yi Xing,Xing Yuan,Jiao Qu
A hierarchically photocatalytic microbial fuel cell system (PMFC) coupled with TiO 2 photoanode and bioanode was established to enhance the power generation based on single-chamber MFC. Compared with the conventional anaerobic mode, oxygen in the solution could be utilized by the photoanode of PMFC to improve the removal of o-chlorophenol (2-CP). The maximum power densities were increasing from 261 (MFC) to 301 mW/m 2 (PMFC). The removal efficiency of 2-CP (5 mg/L) in PMFC was 76.20% and higher than that in MFC (19.33%) and by photocatalysis (49.23%). The electron-hole separation efficiencies were decreasing with the increasing of dissolved oxygen, causing a low efficiency of photocatalysis, due to the reduction of the current density of the systems. The abundance of Geobacter sp., PHOS-HE36 fam., and Pseudomonas sp. was increased with illumination, contributing to improve the electricity production and 2-CP degradation. The only detective intermediate of 1,2-dichlorobenzene in PMFC indicated that the microbes could regulate the degradation pathway of 2-CP in the coupling system. These findings provided an feasible method for the effective degradation of refractory organic compounds and simultaneous energy recovery by combining photocatalysis and microbial power generation.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2022
·
IF 4.598
Qiankun Zhang,Tao Shao,Yu Li,Dehong Bai,Ziyu Xue,Shijie He,Dongxia Zhang,Xibin Zhou
Control of the chemical composition and morphology of electrochemical nanocatalysts is a promising strategy to effectively promote electrocatalytic oxidation in direct methanol fuel cells (DMFCs). Here, we describe a general soft-template-directed one-pot synthesis for the formation of bimetallic mesoporous nanospheres (MNSs) with cylindrically open mesoporous nanochannels. Three-dimensional (3D) well-dispersed bimetallic PtPd MNSs were prepared through in situ co-reduction of Pt and Pd precursor on the soft-templating structural directing amphiphilic surfactant of bisoctyl dimethyl ammonium chloride (BDAC) under optimal reaction conditions without using any toxic organic solvent. Owing to the synergistic advantages in structure and composition, the as-prepared mesoporous morphology of the bimetallic PtPd MNSs has more active sites and accelerates electron/mass transfer. Especially, the Pt 1 Pd 4.8 MNSs possessed a mass activity of 3450 mA mg metal −1 and specific activity of 163.8 mA cm −2 , which are 6.63 and 20.76 times higher than commercial Pt/C (520 mA mg Pt −1 and 7.89 mA cm −2 ). Therefore, it shows outstanding catalytic activity and stability toward electrocatalytic oxidation of methanol under alkaline conditions.
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JOURNAL OF NANOPARTICLE RESEARCH
·
2022
·Vol. 24
·期 3
·1-22
·
IF 2.533
Yang Chunyan,Xue Ziwei,Yin Hao,Lu Ke,Liu Wei
In this work, the photodegradation of methylene blue was investigated by constructing a novel photocatalysis reactor, which was filled with aqueous foam. Nanoscale TiO 2 particles were used as photocatalyst. In order to obtain stable foam phase, cetyl trimethyl ammonium bromide (CTAB) was used as the frother, and its suitable initial concentration in the feeding solution was 0.20 g/L. Under the suitable conditions of loading liquid volume 200 mL, initial concentration of TiO 2 nano-catalysts in the feeding solution 5.0 g/L, inner diameter of foam column 18 mm, aperture diameter of gas distributor 125 μm, and circulating velocity of bulk solution 500 mL/h, the maximum degradation percentage of methylene blue was 97.6 ± 1.2%. Atomic force microscopy (AFM) analysis suggested that the entrainment effect of rising bubbles and the circulation flow of bulk solution inside the aqueous foam did not cause the conspicuous aggregation of TiO 2 nano-catalysts under the suitable conditions, but their surface roughness decreased. Meanwhile, foam entrainment had not a significant impact on the polydispersity of TiO 2 nano-catalysts. In contrast to the photodegradation of methylene blue in aqueous solution, the photocatalysis process using aqueous foam is the intensity of light received by TiO 2 nano-catalyst increases, and irradiation period is less. This work is expected to provide new insight into the rational design of photocatalysis reactor, to facilitate the harmless treatment of dyestuff wastewater. Graphical abstract
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危险品化学品经营许可证（带存储）