INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2026
·
IF 9.2
Dan Zhang,Jin Liu,Bin Song,Chenyu Li,Yuyao Chen,Huaifang Zhang,Yuanyuan Feng
“Time-amount” precise phosphidation successfully constructs amorphous/crystalline/metallic three-phase heterojunction. • Multiphase heterojunction functional synergy facilitates the spatial division of labor for HER pathway at the nanoscale. • Ru→Ru 2 P→a-Ru 2 P relay electron transfer mechanism ensures its excellent seawater HER at industrial current density. Sluggish water dissociation kinetics and stability issues caused by chloride ions pose severe challenges for hydrogen evolution reaction (HER) catalysts in alkaline seawater environments. This study proposes a design philosophy of “multiphase heterojunction functional synergy”. Through a precise microwave phosphidation strategy, a three-phase heterojunction catalyst composed of amorphous Ru 2 P, crystalline Ru 2 P, and metallic Ru (a/c-Ru 2 P@Ru/C) was successfully synthesized. Systematic modulation enabled controllable synthesis of the catalyst's microstructure (amorphous/crystalline phase ratio) and macroscopic composition. This catalyst demonstrates outstanding comprehensive performance in alkaline seawater media: it exhibits a low overpotential of only 36 mV at a current density of 10 mA cm −2 , maintains stable operation for over 200 h at a high current density of 500 mA cm −2 , and shows leading cell voltage for overall water splitting. A series of characterizations indicate that the successful formation of a three-phase heterostructure in a/c-Ru 2 P@Ru/C induces interfacial electron transfer from Ru to phosphides, thereby optimizing the electronic structure of active sites. This multiphase synergy achieves a “spatial division of labor” in the HER reaction pathway: electron-rich amorphous regions promote water dissociation, while electron-modulated metallic sites accelerate hydrogen desorption. Concurrently, the robust heterointerface ensures long-term stability under harsh seawater conditions.
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-11
·
IF 16.6
Zhang Rong,Li Chuan,Cui Huilin,Wang Yanbo,Zhang Shaoce,Li Pei,Hou Yue,Guo Ying,Liang Guojin,Huang Zhaodong,Peng Chao,Zhi Chunyi
Most current research is devoted to electrochemical nitrate reduction reaction for ammonia synthesis under alkaline/neutral media while the investigation of nitrate reduction under acidic conditions is rarely reported. In this work, we demonstrate the potential of TiO 2 nanosheet with intrinsically poor hydrogen-evolution activity for selective and rapid nitrate reduction to ammonia under acidic conditions. Hybridized with iron phthalocyanine, the resulting catalyst displays remarkably improved efficiency toward ammonia formation owing to the enhanced nitrate adsorption, suppressed hydrogen evolution and lowered energy barrier for the rate-determining step. Then, an alkaline-acid hybrid Zn-nitrate battery was developed with high open-circuit voltage of 1.99 V and power density of 91.4 mW cm –2 . Further, the environmental sulfur recovery can be powered by above hybrid battery and the hydrazine-nitrate fuel cell can be developed for simultaneously hydrazine/nitrate conversion and electricity generation. This work demonstrates the attractive potential of acidic nitrate reduction for ammonia electrosynthesis and broadens the field of energy conversion.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Changyu Zhang,Jingchun Jia,Ying Chang,Shaohong Guo,Meilin Jia
Platinum-based alloy catalysts have been extensively studied in the oxygen reduction reaction (ORR) because of their excellent performance. In this study, Pt 5 Ce–CeO 2 /C composite catalysts were synthesized by polyol reduction method and high-temperature calcination method. Owing to the dual effects of the alloying effect of forming Pt 5 Ce intermetallic compound and the electronic effect of CeO 2 modulating the electronic structure of Pt, it exhibits further improved ORR performance than the commercial Pt/C catalysts. The material possesses a 1.0 V starting potential, a 0.83 V half-wave potential, high durability, and methanol resistance. It has strong ORR catalytic activity and works well in Zn-air batteries. The experimental findings demonstrate that metal oxide and alloy structure can be combined to enhance catalyst ORR performance.
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MOLECULES
·
2023
·Vol. 28
·期 20
·7147
·
IF 4.6
Xiafei Gao,Mengyue Gao,Xueping Yu,Xiaoyong Jin,Gang Ni,Juan Peng
The very slow anodic oxygen evolution reaction (OER) greatly limits the development of large-scale hydrogen production via water electrolysis. By replacing OER with an easier urea oxidation reaction (UOR), developing an HER/UOR coupling electrolysis system for hydrogen production could save a significant amount of energy and money. An Al-doped cobalt ferrocyanide (Al-Co2Fe(CN)6) nanocube array was in situ grown on nickel foam (Al-Co2Fe(CN)6/NF). Due to the unique nanocube array structure and regulated electronic structure of Al-Co2Fe(CN)6, the as-prepared Al-Co2Fe(CN)6/NF electrode exhibited outstanding catalytic activities and long-term stability to both UOR and HER. The Al-Co2Fe(CN)6/NF electrode needed potentials of 0.169 V and 1.118 V (vs. a reversible hydrogen electrode) to drive 10 mA cm−2for HER and UOR, respectively, in alkaline conditions. Applying the Al-Co2Fe(CN)6/NF to a whole-urea electrolysis system, 10 mA cm−2was achieved at a cell voltage of 1.357 V, which saved 11.2% electricity energy compared to that of traditional water splitting. Density functional theory calculations demonstrated that the boosted UOR activity comes from Co sites with Al-doped electronic environments. This promoted and balanced the adsorption/desorption of the main intermediates in the UOR process. This work indicates that Co-based materials as efficient catalysts have great prospects for application in urea electrolysis systems and are expected to achieve low-cost and energy-saving H2production.Keywords:hydrogen;urea oxidation;electronic structure;energy-saving;cobalt ferrocyanide
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Yanqing Wei,Yize Zhao,Yue Liu,Na Luo,Zunchang Gao,Pu Hou,Yang Liu,Yanhua Zhang,Pengfei Huo
Nanochannel ionic diodes require extremely complex and expensive fabrication processes. Polyelectrolyte ionic diodes attracted widespread attention among ionic rectification systems due to their simplicity of development and the ability to break the size limits of the nanochannel. However, enhancement of their rectification ratio is still in the exploratory stage. In this study, chitosan (CS) hydrogels and sodium polyacrylate (PAAs) hydrogels were prepared as the substrates for the heterostructured ionic diodes. 5,10,15,20-Tetrakis(4-aminophenyl)-21H,23H-porphyrin (TAPP) was selected to regulate the rectification ratio of ionic diodes. By adding 0.05 wt % TAPP to the CS hydrogel, the rectification ratio of the ionic diode can be increased to 10, which is 4 times larger than that of the undoped ionic diode. In contrast, the rectification ratio of the ionic diodes with TAPP added in the PAAs hydrogel decreases to 2. In addition, the ionic diode composed of the TAPP-doped CS hydrogel and PAAs hydrogel has the characteristics of a high open-circuit voltage. The open-circuit voltage of the 10 mm × 10 mm × 4 mm heterojunction hydrogel reached 370 mV. The ionic diodes can be used as a self-powered power supply device.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Rui Feng,Qi-Dong Ruan,Jiu-Ju Feng,You-Qiang Yao,Lin-Mei Li,Lu Zhang,Ai-Jun Wang
Single-atom transition metal-based nitrogen-doped carbon (M−N x −C) is regarded as high-efficiency and cost-effectiveness alternatives to replace noble metal catalysts for oxygen reduction reaction (ORR) in renewable energy storage and conversion devices. In this work, rich FeCo dual-single atoms were efficiently entrapped into N -doped carbon nanocages (FeCo DSAs-NCCs) by simple pyrolysis of the bimetallic precursors doped zeolitic imidazolate framework-8 (ZIF-8), as affirmed by a series of characterizations. The graphitization degree of the N -doping carbon substrate was regulated by modulating the pyrolysis temperature and the types of the metal salts. The typical catalyst substantially improved the alkaline ORR performance, with the onset potential ( E onset ) of 0.99 V ( vs . RHE) and half-wave potential ( E 1/2 ) of 0.88 V ( vs . RHE). Ultimately, the catalyst-assembled Zn-air battery possessed a higher open-circuit voltage of 1.501 V, larger power density of 123.7 mW cm −2 , and outstanding durability for 150 h. This study provides a guide on developing ORR catalysts for electrochemical energy conversion and storage technology.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Wenfang Zhai,Yuting He,Yu-e Duan,Shengwu Guo,Yuanzhen Chen,Zhengfei Dai,Liting Liu,Qiang Tan
The fundamental challenge of trimetallic single-atoms catalysts stems from the difficulty in supporting the coexistence of different metals with their unique physicochemical features. Here, the trimetallic single-atoms electrocatalyst is constructed as a model system to explore electrocatalytic ORR/OER. The tri-metal (Fe, Co, and Ni) single-atoms loaded on nitrogen-carbon framework exhibits superior ORR/OER kinetics (E 1/2 = 0.927 V, E j =10 = 1.56 V). The flexible zinc-air batteries generate excellent power density and durability (62 mW cm −2 and 200 h at −15 °C, 291.2 mW cm −2 and 250 h at room temperature). Density functional calculations confirm that the trimetallic synergy effect outperform mono- and bimetallic effects, yielding adsorption strength close to 0. This paper describes an intuitionistic descriptor where ΔE OH* displays a volcano relationship with ORR overpotential, and establishes a generalized strategy for efficient bifunctional oxygen electrocatalyst while comprehensively understanding the structure-mechanism-activity relationship.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Can-Wen Yu,Cong-Yi Du,Ting Ouyang,Xi-Ting Zhang,Zhao-Qing Liu
Physical structure change of catalysts based on the electronic metal-support interaction (EMSI) effects is a prospective strategy to regulate the surface electronic structure of catalysts and further enhance their catalytic performance. To optimize the constrained intrinsic oxygen evolution reaction/oxygen reduction reaction (OER/ORR) activity of spinel MnCo 2 O 4 , we present a facile hydrothermal and photoreduction strategy to synthesize the Ag and MnCo 2 O 4 supported on N-doped carbon nanotubes (Ag-MnCoO/NCNTs) with the EMSI effect. Ag-MnCoO/NCNTs as catalyst shows enhanced performance for OER (overpotential of 340 mV) and ORR (half-wave potential of 0.80 V). Furthermore, a zinc-air battery is assembled based on Ag-MnCoO/NCNTs cathode, which affords an open circuit potential of 1.49 V and favorable cycling performance for 200 h. Theoretical calculations illustrate the introduction of Ag reduces the charge density of the tetrahedral Co site along the direction of the dangling bonds and optimizes the adsorption of oxygen intermediates on tetrahedral Co, thus lowering the reaction activation energy and improving its oxygen catalytic activity. This work provides new insights to guide the fabrication of advanced oxygen electrocatalysts.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Jialin Cai,Wenlei Zhang,Yanyan Liu,Ruofan Shen,Xin Xie,Wanyu Tian,Xingang Zhang,Jie Ding,Yushan Liu,Baojun Li
The development of high-efficiency pH-universal electrocatalyst is of great significance for hydrogen evolution reaction (HER). In this work, a rod-like Ru/WO 3 -V O electrocatalyst was constructed for HER via a solid-phase reaction strategy. Due to the restriction of atomic migration at solid phase interface, plenty of oxygen vacancies (V O ) and structure distortions were generated in amorphous/crystalline WO 3 phase (WO 3 -V O ). The optimized Ru/WO 3 -V O annealed at 450 °C with 2.2 wt % Ru achieves outstanding intrinsic activity with low overpotential and Tafel slope in a 0–14 pH range. A turnover frequency value 7.2 higher than that of commercial Pt/C is abtaind on Ru/WO 3 -V O at overpotential of 100 mV. Density functional theory calculations reveal that H* adsorption and desorption balanced by tuning the interface electronic structure contributes synergistic effect to the pH-universal HER activity of Ru/WO 3 -V O . The crystalline/amorphous semiconductor-metal heterointerface is crucial to designing and synthesizing electrocatalysts for optimal HER activity.
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DALTON TRANSACTIONS
·
2023
·Vol. 52
·期 47
·17826-17833
·
IF 4
Yixuan Li,Peiyan Li,Jiahui Jiang,Ting Zhao,Guancheng Xu,Li Zhang
A self-derivation strategy using conductive substrates is used to prepare one-piece highly efficient bifunctional electrodes, where the chosen substrate acts as both an active catalyst precursor and a conductive carrier. Here, a bifunctional catalyst, porous NiS/Ni9S8/NF-2 nanorods, was synthesized by low-temperature vulcanization after an oxalic acid etching process. To reach a current density of 10 mA cm−2, NiS/Ni9S8/NF-2 requires only a tiny overpotential of 115 mV for the HER and 176 mV for the OER, and demonstrates sustained activity for 100 hours with almost any degradation. The substrate self-derived NiS/Ni9S8/NF-2 catalyst for overall water splitting requires only a small voltage of 1.52 V to deliver 10 mA cm−2 with excellent stability. Experimental results show that the heterostructured electrocatalysts impart good catalytic properties of NiS/Ni9S8/NF-2 by modulating the electronic structure and promoting the reconstruction process from sulfides to hydroxides. This work demonstrates the success of the substrate self-derivation strategy to achieve high catalytic activity and provide a new autogenous growth technique for electrode fabrication.
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APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Jundan Tang,Lihua Shen,Kunpeng Zhao,Jiaming Peng,Qili Chen,Chunxia Yu,Yuangang Li,Azhar Abbas,Shan Wang,Zhifang Liu
Nanomaterials-based gas sensors are conducive to online, real-time monitoring and large-scale production due to their simplicity, low energy consumption and miniaturization. Conventional nanomaterial-based (metal oxide semiconductor or two-dimensional nanomaterials) gas sensors are less sensitive (ppm-ppb level). So, it is significantly meaningful to develop new gas-sensing materials. Herein, Ag@sulfur nanosheets (S-NSs) nanocomposite-based sensor is explored for ultrasensitive detection of NH 3 in dry air at room temperature at parts per trillion (ppt) level. Introducing Ag nanoparticles (NPs) on S-NSs, improved electrical conductivity and created more effective adsorption sites, leading to a high response rate of 1.92 for 3 ppt NH 3 . The developed Ag@ S-NSs sensor showed a linear response to NH 3 in the range of 3–70 ppt with correlation coefficient of 0.996. Moreover, the developed Ag@S-NSs sensor showed fast response and recovery time (28/7 s) to NH 3 . The probable sensing mechanism is supposed that the polarization-induction of NH 3 changed of electronic energy level of Ag@S-NSs, and the changed energy is at approximately the same energy level of the Ag@S-NSs itself. Thus, a response signal caused by NH 3 with low concentration can also be felt by Ag@S-NSs sensing materials itself.
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Materials Horizons
·
2023
·Vol. 10
·期 12
·5847-5858
·
IF 13.3
Guosheng Jia,Yan Yu,Xuefen Wang,Chao Jia,Zexu Hu,Senlong Yu,Hengxue Xiang,Meifang Zhu
Bio-based carbon fibers derived from lignin have gained significant attention due to their diverse and renewable sources, ease of extraction, and low cost. However, the current limitations of low specific surface area and insufficient electrical conductivity hinder the widespread application of lignin-derived carbon fibers (LCFs). In this work, highly conductive and porous LCFs are developed through melt-blowing, pretreatment, and carbonization processes. The effects of the carbonization temperature and heating rate on the structures and properties of the LCFs are systematically investigated. The resultant LCFs exhibit high electrical conductivity (71 400 S m−1) and a large specific surface area (923 m2 g−1). The assembled lithium-ion battery based on the LCF anodes demonstrates a long cycle life of >800 cycles and a high specific capacity of 466 mA h g−1. The findings of this study hold practical significance for promoting the utilization of lignin in the fields of energy storage, adsorption, and beyond.
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