JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
·
IF 9.7
Junzheng Jiang,Yunfan Qiu,Hao Dong,Lei Yang,Yaping Miao,Liwei Xiong,Biao Gao,Xuming Zhang,Paul K. Chu,Xiang Peng
Molybdenum nitrides have garnered significant attention for their potential in the hydrogen evolution reaction (HER) due to their metallic behavior, abundant reserves, and pH-universal stability. However, their unsatisfactory hydrogen adsorption limits industrial applications. Heterostructures can be designed to introduce defects and modulate the electronic structure of catalysts to optimize hydrogen adsorption to enhance HER. Nevertheless, the exact active sites at the heterointerface and the fundamental mechanisms underlying the HER process remain inadequately understood. Herein, a composite electrocatalyst in which metallic Ni and MoN phases (Ni/MoN) form the heterointerface between them is fabricated. The heterointerface produces strong electronic interactions between Ni and MoN to facilitate electron transfer from MoN to Ni, and the built-in electric field facilitates charge transfer during electrocatalysis. This optimized electronic configuration with abundant active sites delivers excellent performance in alkaline HER. Density-functional theory calculations demonstrate that H 2 O dissociates at the Ni site, whereas H 2 desorption occurs at the Mo site. As a result, Ni/MoN/CC requires an overpotential of only 95 mV to achieve a current density of 10 mA cm −2 and a Tafel slope of 104 mV dec −1 . Moreover, it maintains a high current density of 100 mA cm −2 for 100 h with negligible morphological or compositional changes. The strategy of modulating the electronic structure of low-cost, transition metal-based heterostructured electrocatalysts is an effective and commercially viable means to design and develop high-performance electrocatalysts for water splitting.
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Journal of Energy Chemistry
·
2024
·
IF 14
Minmin Wang,Chao Feng,Xin Zhang,Ping He,Houyu Zhu,Yunqi Liu,Yuan Pan
The development of atomically dispersed platinum-based catalysts with high performance and well-defined active site structures is crucial for the commercialization of water electrolysis for hydrogen production. Herein, we propose a coordination dual-shell synergistic regulation mechanism of coal pitch-derived carbon-supported single atom Pt-N x O y -S 1 catalytic sites by a self-assembly-pyrolysis strategy for promoting hydrogen evolution reaction (HER). The Pt-N 3 O 1 -S 1 sites exhibited the highest HER performance, with an overpotential of 92 mV at a current density of 400 mA cm −2 . At 50 mV, the turnover frequency was 34.04 s −1 and the mass activity was 22.83 A mg Pt −1 , which is 63.4 times that of the 20% Pt/C catalyst. Theoretical calculations revealed that the coordination dual-shell impacts the electronic structure of the Pt atoms and the adsorption strength towards reactants synergistically. The S atoms in the second coordination shell weakened the strength of Pt-N first shell, resulting the more surface valence electrons around Pt atoms, exhibiting the most suitable adsorption free energy and enhancing the adsorption of H + on Pt-N 3 O 1 -S 1 sites, thus enhancing the electrocatalytic HER process by promoting Volmer step. This work reveals that coordination dual-shell synergistic regulation is an effective strategy for enhancing the electrocatalytic reaction process.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Jiayun Song,Zixiao Li,Shengjun Sun,Chaoxin Yang,Zhengwei Cai,Xiaoyan Wang,Meng Yue,Min Zhang,Hefeng Wang,Asmaa Farouk,Mohamed S. Hamdy,Xuping Sun,Bo Tang
Seawater electrolysis taking advantage of coastal/offshore areas is acknowledged as a potential way of large-scale producing H 2 to substitute traditional technology. However, anodic catalysts with high overpotentials and limited lifespans (caused by chloride-induced competitive chemical reactions) hinder the system of seawater electrolysis for H 2 production. Herein, we present a citrate anion (CA) modified NiFe layered double hydroxide nanosheet array on nickel foam (NiFe LDH@NiFe-CA/NF), which serves as an efficient and stable electrocatalyst towards long-term alkaline seawater oxidation. It requires only a low overpotential of 387 mV to achieve a current density of 1000 mA cm −2 , outperforming NiFe LDH/NF (414 mV). Moreover, NiFe LDH@NiFe-CA/NF exhibits continuous oxygen evolution testing for 300 h at 1000 mA cm −2 due to its anti-corrosion characterization. Additionally, the fabricated cell can stably operate at 300 mA cm −2 (60 °C, 6 M KOH + seawater) and only require 1.69 V, achieving low energy consumption of seawater splitting.
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Inorganic Chemistry Frontiers
·
2024
·Vol. 11
·期 20
·6909-6918
·
IF 6.1
Hongjun Chen,Liming Deng,Sheng Zhao,Shuyi Liu,Feng Hu,Linlin Li,Jianwei Ren,Shengjie Peng
Developing efficient and durable hydrogen evolution reaction (HER) electrocatalysts is critical for industrial and sustainable hydrogen production. Herein, a simple co-precipitation strategy is proposed to successfully construct catalysts with a Mott–Schottky heterojunction by coupling a transition-metal phosphate to the surface of stripped MXene thin-layer nanosheets (M3(PO4)2@MXene, M = Co, Ni, and Fe). The Co3(PO4)2@MXene with a unique tightly connected 2D/2D heterostructure and built-in electric field induces directional electron transfer at the interface, regulates the polarized structure of the active sites, and accelerates both mass and electron transport. Consequently, the optimized Co3(PO4)2@MXene demonstrates outstanding HER performance, achieving low overpotentials of 46 and 58.6 mV at 10 mA cm−2 in alkaline freshwater and seawater electrolytes, respectively. Moreover, the Co3(PO4)2@MXene heterojunction catalyst maintains stable operation at a high current density of 500 mA cm−2 for over 100 h in alkaline seawater electrolytes. More importantly, Co3(PO4)2@MXene can offer a low potential of 1.71 V at 500 mA cm−2 with stable operation for 50 h in a flow-type alkaline seawater electrolyser. This study provides a unique heterostructure in an electrocatalyst for an efficient HER and presents its potential application in seawater electrolysis.
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Small
·
2024
·
IF 13
Huamei Tong,Shengjie Xu,Xinyu Zheng,Mengyue Qi,Jianjun Zhu,Di Li,Deli Jiang
Constructing metal alloys/metal oxides heterostructured electrocatalysts with abundant and strongly coupling interfaces is vital yet challenging for practical electrocatalytic water splitting. Herein, CoRu nanoalloys uniformly anchored on CoMoO 4 nanosheet heterostructured electrocatalyst (CoRu-CoMoO 4 /NF) are synthesized via a self-templated strategy by simply annealing of Ru-etched CoMoO 4 /NF precursor in a reduction atmosphere. The dense and robustly coupled interface not only provides abundant active sites for water splitting but also strengthens the charge transfer efficiency. Furthermore, the theoretical calculations unveil that the strong electronic interaction at CoRu-CoMoO 4 interface can induce an interfacial electron redistribution and reduce the energetic barriers for the hydrogen and oxygen intermediates, thereby accelerating the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) kinetics. The resultant catalyst only requires the overpotentials of 49 mV for HER and 209 mV for OER at 10 mA cm −2 . Moreover, the constructed CoRu-CoMoO 4 ||CoRu-CoMoO 4 two-electrode cell achieves a cell voltage of 1.54 V at 10 mA cm −2 , outperforming the benchmark Pt/C||IrO 2 . This work explores an avenue for the rational design of heterostructured electrocatalysts with abundant interfaces for practical water-splitting electrocatalysis.
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INORGANIC CHEMISTRY
·
2024
·
IF 4.3
Xiaofeng Lin,Shuli Tang,Min Yang,Zhiqiang Zhang,Qitong Huang
Exploration of electrocatalysts suitable for the oxygen evolution reaction (OER) and urea oxidation reaction (UOR) is essential for electrocatalytic hydrogen production. In this work, a ligand substitution strategy is used to synthesize ultrathin-nanosheet electrocatalysts of Cl-doped NiSe2 (NiSe2-a and NiSe2-b), which exhibit high-electrocatalytic activity during OER and UOR. NiSe2-a and NiSe2-b only need an overpotential of 227 and 268 mV, respectively, to achieve a current density of 10 mA cm–2 during OER. Furthermore, NiSe2-a with its smaller steric effects exhibits excellent catalytic performance for UOR, requiring an ultralow potential of 1.360 V to deliver a current density of 100 mA cm–2. This excellent performance can be attributed to the nonmetallic elements (Se and Cl) modulating and optimizing the charge state of the metal sites, thereby increasing the electrocatalytic activity. Overall, this work provides an unparalleled example of tuning space structures to design efficient electrocatalysts and has promising industrial applications.
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Journal of Materials Chemistry A
·
2025
·
IF 9.5
Yupei Ding,Jie Zhu,Minxia Jiang,Xiaowan Zhan,Jinwen Qin,Xue Jiang,Shuaifeng Wang,Tao Meng,Minhua Cao
RuSe2 has been considered an efficient alkaline hydrogen evolution reaction (HER) electrocatalyst due to its fast water dissociation kinetics and lower price. However, its strong affinity to the adsorbed active intermediates blocks the active sites, hence largely falling short of its full activity potential. Herein, we report a feasible competitive adsorption strategy by introducing oxyphilic molybdenum (Mo) species into RuSe2 (Mo–RuSe2) to regulate the strong interaction between the Ru sites and HER intermediates, enabling highly efficient alkaline HER performance. In situ experimental and theoretical calculation results reveal that the oxyphilic Mo tailoring for RuSe2 can not only alleviate OHad blocking on the Ru sites by the competitive adsorption of OHad between the Ru and Mo sites, but also optimize the hydrogen adsorption Gibbs free energy, thus facilitating the OHad transfer and H2 release process, both of which synergistically promote the regeneration of Ru active sites. The optimized Mo–RuSe2 exhibits an overpotential at 10 mA cm−2 as small as 27 mV and a low Tafel slope of 39 mV dec−1, as well as remarkable long-term stability. This finding is expected to shed new light on developing highly efficient alkaline HER catalysts by regulating the adsorption strength between the active sites and intermediates.
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ELECTROCHIMICA ACTA
·
2017
·
IF 4.798
Ruijing Wang,Peng Sun,Huanwen Wang,Xuefeng Wang
At high current density during the hydrogen evolution reaction (HER) process, the active layer for most of MoS 2 -based electrocatalysts suffers from pulverizations and easily drops-off due to a high rate of bubble formation and strong stirring. Herein, a facile pulsed laser deposition (PLD) method is used to fabricate amorphous molybdenum disulfide (MoS 2 ) films on gold-coated carbon cloth (Au/CC) for HER test. Because of the strong anchoring interaction between MoS 2 catalysts and the Au/CC substrate during the underlying laser ablation process, remarkable stability with 5000 continuous HER cycles has been achieved in the acid media. Furthermore, the as-obtained MoS 2 catalyst shows a small Tafel slope of 48 mV decade −1 , an onset overpotential of 132 mV and the overpotential of 180 mV at a current density of 10 mA cm −2 . These results demonstrate that PLD is a very promising technique for making the film electrodes for application in electrocatalytic process.
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Materials
·
2017
·Vol. 10
·期 5
·564
·
IF 2.654
Wensheng Li,Lingtao Sun,Rong Hu,Wenli Liao,Zhongbin Li,Yanrong Li,Chaozhong Guo
The great challenge of boosting the oxygen reduction reaction (ORR) activity of non-noble-metal electrocatalysts is how to achieve effective exposure and full utilization of nitrogen-rich active sites. To realize the goals of high utilization of active sites and fast electron transport, here we report a new strategy for synthesis of an iron and nitrogen co-doped carbon nanolayers-wrapped multi-walled carbon nanotubes as ORR electrocatalyst (N-C@CNT-Fe) via using partially carbonized hemoglobin as a single-source precursor. The onset and half-wave potentials for ORR of N-C@CNT-Fe are only 45 and 54 mV lower than those on a commercial Pt/C (20 wt.% Pt) catalyst, respectively. Besides, this catalyst prepared in this work has been confirmed to follow a four-electron reaction mechanism in ORR process, and also displays ultra-high electrochemical cycling stability in both acidic and alkaline electrolytes. The enhancement of ORR activity can be not only attributed to full exposure and utilization of active site structures, but also can be resulted from the improvement of electrical conductivity owing to the introduction of CNT support. The analysis of X-ray photoelectric spectroscopy shows that both Fe–N and graphitic-N species may be the ORR active site structures of the prepared catalyst. Our study can provide a valuable idea for effective improvement of the electrocatalytic activity of non-noble-metal ORR catalysts.Keywords:oxygen reduction;electrocatalyst;active site;carbon nanotube;hemoglobin
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Journal of Energy Chemistry
·
2024
·
IF 14
Yongchao Yao,Shengjun Sun,Hui Zhang,Zixiao Li,Chaoxin Yang,Zhengwei Cai,Xun He,Kai Dong,Yonglan Luo,Yan Wang,Yuchun Ren,Qian Liu,Dongdong Zheng,Weihua Zhuang,Bo Tang,Xuping Sun,Wenchuang (Walter) Hu
Electrocatalytic hydrogen production from seawater holds enormous promise for clean energy generation. Nevertheless, the direct electrolysis of seawater encounters significant challenges due to poor anodic stability caused by detrimental chlorine chemistry. Herein, we present our recent discovery that the incorporation of Ce into NiFe layered double hydroxide nanosheet array on Ni foam (Ce-NiFe LDH/NF) emerges as a robust electrocatalyst for seawater oxidation. During the seawater oxidation process, CeO 2 is generated, effectively repelling Cl − and inhibiting the formation of ClO − , resulting in a notable enhancement in the oxidation activity and stability of alkaline seawater. The prepared Ce-NiFe LDH/NF requires only overpotential of 390 mV to achieve the current density of 1 A cm −2 , while maintaining long-term stability for 500 h, outperforming the performance of NiFe LDH/NF (430 mV, 150 h) by a significant margin. This study highlights the effectiveness of a Ce-doping strategy in augmenting the activity and stability of materials based on NiFe LDH in seawater electrolysis for oxygen evolution.
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APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Jiapeng Wang,Xinpeng Chen,Hua-Bin Yuan,Lili Xing,Desheng Sha,Aijing Li,Guoqiang Chen,Tieling Xing
Metal-organic frameworks (MOFs) find wide-ranging applications owing to their adjustable structures, diverse compositions, and large specific surface area. In this work, MOFs materials were grown in situ on carbon cloth, yielding self-supported electrodes V O -(Fe,Co) 3 O 4 @CC rich in oxygen vacancies through a simple high-temperature annealing treatment utilizing NaBH 4 as an etchant. Thus the resulting self-supported electrode V O -(Fe,Co) 3 O 4 @CC exhibited excellent oxygen evolution reaction (OER) performance, achieving an overpotential of merely 288 mV at 10 mA cm −2 , along with a low Tafel slope of 31.39 mV dec -1 , and demonstrating robust long-term activity and stability. In addition, a liquid zinc-air battery was assembled utilizing the prepared V O -(Fe,Co) 3 O 4 @CC as an air cathode, achieving a high open-circuit voltage of 1.46 V and a high peak power density of 89.06 mW cm −2 , and it maintained excellent cycling stability during cyclic charging and discharging (with a current density of 2 mA cm −2 ) over a 32 h period. Meanwhile, the self-supported electrode V O -(Fe,Co) 3 O 4 @CC served as an air cathode for assembling an all-solid-state flexible zinc-air battery (ZAB), demonstrating a high peak power density (38.21 mW cm −2 ) and exhibiting favorable cycling stability. This experiment offers insights into the potential application of MOF-derived electrocatalysts in water decomposition and zinc-air batteries.
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NEW JOURNAL OF CHEMISTRY
·
2024
·Vol. 48
·期 48
·20351-20357
·
IF 2.7
Mengyu Hu,Hanzhi Yu,Chong Chen,Yukun Zhang,Changjiang Hu,Jun Ma
The development of anodic reactions with accelerated kinetics to replace the oxygen evolution reaction (OER) to promote the hydrogen evolution reaction (HER) with high value-added production is of crucial importance in the field of electrocatalytic hydrogen production. In this paper, the thermodynamically favourable methanol oxidation reaction (MOR) is combined with the HER for energy-efficient hydrogen production. The Ru nanoparticles supported on metal–organic framework nanolayers (Ru@Co MOLs) are synthesized via a gamma-ray irradiation-induced reduction reaction. The abundant defects within the composite facilitate uniform dispersion and strong anchoring of Ru. As a result, Ru@Co MOLs exhibit remarkable HER and MOR activity with an overpotential of 20 mV and 1.094 V at 10 mA cm−2. Moreover, in the presence of methanol, they only require a lower voltage of 1.182 V at 10 mA cm−2 in a two-electrode electrolyzer. This work presents a promising bifunctional catalyst for methanol oxidation with energy-efficient hydrogen production.
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