INORGANIC CHEMISTRY
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2024
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IF 4.3
Long Qian,Yao Zhu,Huiting Hu,Yunhua Zheng,Ziyu Yuan,Yuting Dai,Tao Zhang,Dongya Yang,Songlin Xue,Fengxian Qiu
Electrochemical water splitting is a possible way of realizing sustainable and clean hydrogen production but is challenging, because a highly active and durable electrocatalyst is essential. In this work, we integrated heterogeneous engineering and vacancy defect strategies to design and fabricate a heterostructure electrocatalyst (CoPv-MoxPv/CNT) with abundant phosphorus vacancies attached to carbon nanotubes (CNTs). The vacancy defects enabled the optimization of the electronic structure; thereby, the electron-rich low-valent metal sites enhanced the ability of nonmetallic P to capture proton H. Meanwhile, the heterogeneous interface between bimetallic phosphides and CNTs realized rapid electron transfer. In addition, the Co, Mo, and P active species in the electrocatalytic process exposed increased amounts of active sites featuring porous nanosheet structures, which facilitated the adsorption of reaction intermediates and thus enhanced the hydrogen evolution reaction performance. In particular, the optimized CoPv-MoxPv/CNT catalyst possesses an overpotential of 138 mV at a current density of 10 mA cm–2 and long-term stability for 24 h. This work offers insights and possibilities for the engineering and exploration of transition metal-based electrocatalysts through combining multiple synergistic strategies.
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Catalysis Science & Technology
·
2024
·Vol. 14
·期 13
·3719-3727
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IF 4.4
Wensheng Zhang,Xu Chen,Jinyu Zhao,Lin Niu,Guipeng Wang,Xiaomin Wang
The potential of hydrogen production via water splitting technology makes it urgent to develop low-cost and highly active bifunctional catalysts for hydrogen and oxygen evolution reactions (HER/OER). In this study, a low platinum (Pt) bimetallic phosphide heterostructure (Pt-NiFe-P/NF), derived from three-dimensional NiFe metal–organic framework (NiFe-MOF) nanorods on nickel foam (NF), was developed using a two-step hydrothermal and phosphorization process. The nickel-iron phosphide nanorod array heterostructure boasts a large surface area with numerous active sites, which enhances charge and substance transfer. The integration of metallic Pt with NiFe-P heterostructures subtly adjusts the electronic redistribution between them, thereby improving the kinetics of water splitting. Consequently, the Pt-NiFe-P/NF catalyst demonstrated exceptional HER and OER performance in a 1 M KOH solution, with overpotentials of 97 and 266 mV at 100 mA cm−2, respectively. Remarkably, an electrolyzer utilizing this catalyst requires just a 1.65 V potential to achieve a current density of 100 mA cm−2, exceeding the capabilities of conventional Pt/C||RuO2 systems, which require 2.10 V and outperforming many advanced electrochemical water splitting catalysts currently in use.
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Xiaojin Yin,Wenhao Xi,Pan Wang,Tongchen Wu,Peide Liu,Bifen Gao,Yun Zheng,Bizhou Lin
It is crucial to develop highly active and durable bifunctional electrocatalysts toward oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) for rechargeable Zn-air batteries. Herein, we report a facile approach to synthesize 2D β-Co(OH) 2 nanosheets supported on 1D nitrogen-doped carbon nanotubes through a hydrothermal in-situ growth strategy of Co nanoparticles encapsulated N-doped carbon nanotubes and urea. The as-obtained Co(OH) 2 /NCNTs displays excellent bifunctional activity with a high half-wave potential of 0.85 V vs. RHE for ORR, a low overpotential of 312 mV at 10 mA cm −2 for OER, and a low potential gap of 0.69 V. Density function theory calculations show that the synergistic effort between doped carbon and β-Co(OH) 2 reduces the energy barriers of the rate determining steps for the former toward ORR and for the latter toward OER, contributing to the superior bifunctional catalytic performance. The assembled Co(OH) 2 /NCNTs- based battery performs a high specific capacity of 883 mAh g Zn -1 and remarkable cycle stability. This presented in-situ construction strategy provides an attractive rational design method for preparing carbon-based bifunctional electrocatalysts.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
·
IF 9.4
Longqian Wang,Pan Wang,Xin Xue,Dan Wang,Huishan Shang,Yafei Zhao,Bing Zhang
Rational designing efficient transition metal-based multifunctional electrocatalysts is highly desirable for improving the efficiency of hydrogen production from water cracking. Herein, a self-supported three-phase heterostructure electrocatalyst of nickel–cobalt sulfide/nickel phosphide/iron phosphide (CoNi 5 S 8 -Ni 2 P-FeP 2 ) was prepared by a two-step gas-phase sulfurization/phosphorization strategy. The heterostructure in CoNi 5 S 8 -Ni 2 P-FeP 2 provides a favorable interfacial environment for electron transfer and synergistic interaction of multiphase active components, while the introduced electronegative P/S not only serves as a carrier for proton capture in the hydrogen evolution reaction (HER) process but also promotes the metal-electron outflow, which in turn accelerates the generation of high-valent Ni 3+ species to enhance the catalytic activity of oxygen evolution reaction (OER) and urea oxidation reaction (UOR). As expected, CoNi 5 S 8 -Ni 2 P-FeP 2 reveals excellent multifunctional electrocatalytic properties. An overpotential of 35/215 mV is required to reach 10 mA cm −2 for HER/OER. More encouragingly, a current of 100 mA cm −2 requires only 1.36 V for UOR with CoNi 5 S 8 -Ni 2 P-FeP 2 as anode, which is much lower as compared to the OER (1.50 V). Besides, a two-electrode water/urea electrolyzer assembled based on CoNi 5 S 8 -Ni 2 P-FeP 2 has a voltage of only 1.59/1.48 V when the system reaches 50 mA cm −2 . This work provides a new idea for the design of energy-efficient water/urea-assisted water-splitting multifunctional catalysts with multi-component heterostructure synergistic interface engineering.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
·
IF 20.2
Houhong Song,Xian Zhou,Xiaofeng Gao,Hantao Gong,Hao Teng,Yongkang Huang,Ziyu Song,Lili Lin,Siyu Yao
Treating and recycling high concentration acetic acid in the exhaust water has long posed a challenge in industry. These wastes containing acetic acid are typically processed via basic neutralization, characterized by high acidity and resistance to degradation, which can bring potential economic burden and environmental hazards. Here we report a new photocatalytic conversion route for addressing high concentrations of acetic acid. This process transforms acetic acid into valuable succinic acid through dehydrogenative coupling. Additionally, the photocatalytic conversion of acetic acid exhibits structure sensitivity when employing Pt cocatalysts of varying sizes. Through inhibiting the undesirable H termination of active free radicals over small Pt atoms and clusters, the rate of undesired decarboxylation reactions can be decreased by 75 %. This effectively enhances the selectivity of the coupling product succinic acid by 2.1 times, achieving a succinic acid formation rate of 7.28 mmol/(g cat •h). This work offers a theoretical guidance for searching value-added reaction pathways of acetic acid, thereby establishing an innovative approach for high concentration exhaust acetic acid treatment and converting low value monocarboxylic molecules into valuable diacid polymerization monomers under a mild and green condition.
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
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2024
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IF 11.2
Qihao Wu,Heju Gao,Jiahui Jiang,Ting Zhao,Shuai Liu,Chunyan Wu,Guancheng Xu,Li Zhang
A flexible air electrode with excellent activity and stability is essential for flexible zinc-air batteries. In this study, we report the rational design of nitrogen-doped carbon nanotube-encapsulated Co 9 S 8 nanoparticles on carbon cloth (Co 9 S 8 /NCNTs/CC), serving as self-supporting air electrodes for both liquid-state and flexible zinc-air batteries. The Co 9 S 8 /NCNTs/CC-1 exhibited a half-wave potential of 0.86 V for oxygen reduction reaction (ORR) and achieved a current density of 10 mA cm −2 for oxygen evolution reaction (OER) at a voltage of only 1.52 V. The well-constructed nanotube on carbon cloth facilitates mass diffusion and electron transfer, while enhancing the mechanical flexibility of the material. Density functional theory (DFT) calculations suggested that the synergistic interaction between Co 9 S 8 and NCNTs effectively enhanced the bifunctional electrocatalytic performance of the material. Liquid-state and flexible zinc-air batteries assembled with Co 9 S 8 /NCNTs/CC-1 demonstrated outstanding charge-discharge capabilities and long-term stability.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
·
IF 8.1
Tong Li,Lingting Ye,Kui Xie
Electrocatalytic full water splitting is still a challenge. Porous single-crystalline (PSC) has a long-range ordered crystal structure and large specific surface area , which has great potential to be applied in the fields of catalysis and energy storage. Nitride single-crystalline possesses unsaturated coordination of metal-nitrogen active sites on the crystal surface, which has shown excellent performance in the electrocatalytic field. PSC tungsten nitride mesoporous nanosheets are grown from single-crystalline (SC) WO 3 nanosheets and are applied as bifunctional electrocatalysts in Hydrogen Evolution Reaction (HER) and Oxygen Evolution Reaction (OER). The overpotential of mesoporous W 2 N and WN single-crystalline nanosheets in HER is as low as 67.44 mV and 84.26 mV at a current density of 10 mA cm −2 , respectively. A low overpotential has been found in PSC W 2 N and WN as the OER electrocatalyst . The PSC tungsten nitride mesoporous nanosheets provide a simple and effective solution for efficient water splitting electrocatalysts .
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Lu Zhang,Ling-Ling Liu,Jiu-Ju Feng,Ai-Jun Wang
Three-dimensional (3D) hollow carbon is one of advanced nanomaterials widely applied in oxygen reduction reaction (ORR). Herein, iron niobate (FeNb 2 O 6 ) nanoparticles supported on metal-organic frameworks (MOFs)-derived 3D N -doped interconnected open carbon cages (FeNb 2 O 6 /NICC) were prepared by methanol induced assembly and pyrolysis strategy. During the fabrication process, the evaporation of methanol promoted the assembly and cross linkage of ZIF-8, rather than individual particles. The assembled ZIF-8 particles worked as in-situ sacrificial templates, in turn forming hierarchically interconnected open carbon cages after high-temperature pyrolysis. The as-made FeNb 2 O 6 /NICC showed a positive onset potential of 1.09 V and a half-wave potential of 0.88 V for the ORR , outperforming commercial Pt/C under the identical conditions. Later on, the as-built Zn-air battery with the FeNb 2 O 6 /NICC presented a greater power density of 100.6 mW cm −2 and durable long-cycle stability by operating for 200 h. For preparing 3D hollow carbon materials, this synthesis does not require a tedious removal process of template, which is more convenient than traditional method with silica and polystyrene spheres as templates. This work affords an exceptional example of developing 3D N -doped interconnected hollow carbon composites for energy conversion and storage devices.
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-12
·
IF 14.7
Ji Qianqian,Tang Bing,Zhang Xilin,Wang Chao,Tan Hao,Zhao Jie,Liu Ruiqi,Sun Mei,Liu Hengjie,Jiang Chang,Zeng Jianrong,Cai Xingke,Yan Wensheng
The microscopic reaction pathway plays a crucial role in determining the electrochemical performance. However, artificially manipulating the reaction pathway still faces considerable challenges. In this study, we focus on the classical acidic water oxidation based on RuO 2 catalysts, which currently face the issues of low activity and poor stability. As a proof-of-concept, we propose a strategy to create local structural symmetry but oxidation-state asymmetric Mn 4-δ -O-Ru 4+δ active sites by introducing Mn atoms into RuO 2 host, thereby switching the reaction pathway from traditional adsorbate evolution mechanism to oxide path mechanism. Through advanced operando synchrotron spectroscopies and density functional theory calculations, we demonstrate the synergistic effect of dual-active metal sites in asymmetric Mn 4-δ -O-Ru 4+δ microstructure in optimizing the adsorption energy and rate-determining step barrier via an oxide path mechanism. This study highlights the importance of engineering reaction pathways and provides an alternative strategy for promoting acidic water oxidation.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Hao Wu,Guoxiang Wang,Xinxin Zhang,Qingwang Min,Jiacheng Wang,Dazhi Wang,Longsheng Cao
Water electrolysis is one of the most promising green hydrogen production technologies. However, using precious metal materials as electrodes for these electrolyzers incurs high costs. To address these challenges and simultaneously retain the catalytic activity of precious metals, we synthesize a low-iridium catalyst, Nd–IrO 2 . At 10 and -10 mA/cm 2 , this catalyst exhibits 233 and 36 mV overpotentials. Nd – IrO 2 maintains stability over prolonged operation in acidic environments, as evidenced by its consistent overpotential. Advanced calculations using density functional theory (DFT) have demonstrated that incorporating Nd and an ample amount of oxygen vacancies can modulate the d-band center of Ir and reduce the adsorption energy of electrochemical reaction intermediates. In summary, we present the synthesis of a low-iridium catalyst, which provides valuable insights for the design and development of catalysts with improved electrocatalytic performance.
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Small
·
2024
·
IF 13
Hongliang Fu,Yue Lian,Yongfeng Hu,Jing Zhao,Huaihao Zhang
The development of highly stable and strongly active electrode materials for sodium-ion batteries (SIBs) and overall water splitting (OWS) is critical in sustainable energy storage and conversion systems. Here, a new electrode material N-Fe-C@Nb 2 CT x is introduced, with a layered sandwich structure consisting of N-doping Fe-MOF derived-nanorods (Fe-C) and Nb 2 CT x MXenes. Specifically, Nb 2 CT x obtained by etching Nb 2 AlC with HF acid is used as the main body to construct the layered sandwich structure with Fe-C as the filler. Benefiting from this structure, Fe-MOF grows in situ within Nb 2 CT x , which restrains MXenes aggregation and stacking and also alleviates the bulk effect of sodium-ion embedding/de-embedding, thus improving its stability. Again, the more exposed active sites from the layered sandwich structure and N-doping introduction ensure high reactivity as electrode materials. In addition, Fe-C nanorods strengthen the linkage between the Nb 2 CT x layers and N-doping enhances the ion/electron transport rate, thereby boosting the effective mass transfer and electrical conductivity. Density functional theory (DFT) calculations show that Fe-C and N-doping help increase the density of states (DOS) and material electrical conductivity. Meanwhile, the generated oxygen species (*OH and *O) in OER are captured by in situ FT-IR test. As a result, the N-Fe-C@Nb 2 CT x electrochemical test displays good electrochemical performance in SIBs and OWS.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Shan Huang,Ling-Xin Kong,Meng-Meng Wang,Hui-Hao Li,Xin-Qi Liu,Meiling Xue,Yi Fang,Ji-Sen Li,Qi Xiao
The electrolysis of seawater for hydrogen production holds promise as a sustainable technology for energy generation. Developing water-splitting catalysts with low overpotential and stable operation in seawater is essential. In this study, we employed a hydrothermal method to synthesize NiMoWO X microrods (NiMoWO X @NF). Subsequently, an annealing process yielded a composite N -doped carbon-coated Ni 3 N/MoO 2 /WO 2 nanorods (NC@Ni 3 N/MoO 2 /WO 2 @NF), preserving the ultrahigh-specific surface area of the original structure. A two-electrode electrolytic cell was assembled using NC@Ni 3 N/MoO 2 /WO 2 @NF as the cathode and NiMoWO X @NF as the anode, demonstrating exceptional performance in seawater splitting. The cell operated at a voltage of 1.51 V with a current density of 100 mA·cm −2 in an alkaline seawater solution. Furthermore, the NC@Ni 3 N/MoO 2 /WO 2 @NF || NiMoWO X @NF electrolytic cell exhibited remarkable stability, running continuously for over 120 h at a current of 1100 mA·cm −2 without any observable delay. These experimental results are corroborated by density functional theory calculations. The NC@Ni 3 N/MoO 2 /WO 2 @NF || NiMoWO X @NF electrolyzer emerges as a promising option for industrial-scale hydrogen production through seawater electrolysis.
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