CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Fanjia Sun,Yanhui Wang,Xueqing Tian,Rui Zhu,Ziliang Zhuang,Youbin Zheng,Jianbing Zang,Liang Dong
Electrocatalysts with high activity and corrosion resistance, tailored for industrial-grade current densities, played a crucial role in seawater electrolysis. Here, we synthesized a petal-like Cr-doped NiFe phosphate 'semi-coated' phosphide heterostructure electrocatalyst grown on nickel foam (Cr-NiFeP/PO 3 @NF). This catalyst demonstrated superior catalytic performance in natural seawater, maintaining stability and only a slight increase in cell voltage after operating continuously for 100 h at a current density of 1 A cm −2 . The incorporation of Cr introduced a significant number of unpaired electrons, which enhanced the conductivity of the catalyst, facilitated the creation of electron depletion regions around Ni and Fe, and improved the interaction with adsorption intermediates. Furthermore, the high activity and corrosion resistance during the oxygen evolution reaction (OER) were due to the interaction between the in-situ formed high-valent phosphate and NiFeCrOOH during the anodization process.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Chuhan Tang,Wei Shan,YiRan Zheng,Liang Zhang,Yuxin Liu,Bin Liao,HeDong Chen,Xianhua Hou
The widespread application of Lithium-ion Batteries (LIBs) has led to a significant increase in the number of spent LIBs. Consequently, the recycling and utilization of spent LIBs have become an inevitable choice for recovering valuable resources and protecting the environment, aligning with the principles of sustainable development. This study reports an iron air battery recycling system that is capable of recovering both Li/Co and energy from spent LiCoO 2 cathode materials and the separation reaction is completely spontaneous. Meanwhile, lithium and cobalt were successfully recovered from the powdered leach solution of spent LiCoO 2 cathode material, and it was preliminarily demonstrated that spent iron could be used as a sacrificial anode for the system. Several key parameters affecting recovery are optimized, including anode solution pH, discharge current density, and concentration of the solution to be recovered. Under the conditions of anode solution pH of 1.8, discharge current density of 0.1 mA cm −2 , and concentration of recovery solution of 0.15 mol/L, the system can be operated stably for more than 24 h, and the recoveries of Li + and Co 2+ can be up to 1.49 mg h −1 and 18.75 mg h −1 respectively, and the output energy can reach 75.15 kJ/mol. This research not only provides a sustainable and cost-effective method of disposing of used lithium-ion batteries, but also offers up new possibilities for the disposal of scrap iron.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Shuai Li,Yimei Zhang
Enhancing the energy efficiency of hydrogen evolution reaction (HER) represents a significant yet challenging goal. One promising approach to achieve this is developing catalysts with high activity and robust stability to couple HER with Fenton reaction. Herein, mesoporous nanosheet arrays (MNA) with featuring a mean pore size of 25 nm, was fabricated via a hydroxide precursor annealing strategy. The produced Co-P MNA 25 and Fe-Co-P MNA 25 are applied in HER and Fenton reaction, respectively. Compared to the MNA 12 synthesized by traditional method of self-growth and solid-phase phosphorization, the MNA 25 exhibited remarkable enhancement in performance, including a 49 % reduction in HER overpotential at 10 mA cm −2 , a 41 % increase in pseudo-first-order degradation kinetics of methylene blue in Fenton reaction, along with superior stability. In addition, the MNA 25 based flow reactor, which couples the two reaction and features a fastener-free design, demands just a minimal voltage of 1.61 V to drive, demonstrating impressive energy efficiency (81.56 % for HER and 2.77 g kWh −1 for Fenton) and application potential. More importantly, numerical simulations reveals that the larger pore size in MNA not only facilitated faster electrolyte diffusion, but also enhanced its impact buffer performance, thereby improving its catalytic activity and stability. Our work unveils the mechanism of mesopore size on the electrochemical performance of catalysts at the theoretical level, which offers a promising avenue for enhancing the energy efficiency of HER.
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CHEMICAL ENGINEERING JOURNAL
·
2024
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IF 13.3
Zhong Wang,Jinzhou Li,Shuang Yuan,Jinshuo Yang,Zhiqiang Jin,Xinjia Tan,Jie Dang,Wangzhong Mu,Guojian Li,Qiang Wang
FeCoNi-based high entropy intermetallic compounds are promising substitutes for noble metal catalysts for hydrogen evolution reaction (HER) and oxygen evolution (OER), while their activity is restricted by the synergistic effect between the elements. In this paper, the theoretical model of FeCoNiMnMoP bifunctional catalyst has been reasonably designed given the volcanic curve of M−H bond energy as a valuable guide for candidate metal elements. Theoretical calculations show that the synergistic effect between multiple sites not only accelerates the electron transfer but also reduces the rate-determining step (RDS) barrier. At the same time, the introduction of Mo also enhances the total density of states and reduces the d-band center, thus optimizing the adsorption and dissociation of intermediates. The experimental results confirm that the theoretical model has excellent catalytic performance. In the alkaline solution, FeCoNiMnMoP‖FeCoNiMnMoP requires only an ultra-low cell voltage of 1.49 V for overall water splitting when the current density is 10 mA cm −2 . In general, novel insights on the effects of intermetallic synergies on water decomposition are provided, which is helpful for the design of bifunctional catalysts based on volcanic diagrams.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Qiusheng Zhou,Minmin Song,Yuan Tian,Min Min,Shiqiang Cui,Xianying He,Chuanyin Xiong
The large-scale application of metal-air batteries strongly depends on the development of cost-effective, highly efficient, and durable bifunctional oxygen catalysts. In this work, a facile approach for preparing the monodisperse PtCo nanoalloy anchored the nitrogen-doped carbon nanotubes (PtCo/NCNT) for zinc-air batteries is reported. The nitrogen-doped carbon shell prevents PtCo nanoalloy from exfoliation, dissolution, and aggregation and enables the accessibility of electrolytes to the alloy surface and the electron transfer. Besides, the strong interaction between PtCo nanoalloy and nitrogen-doped carbon can efficiently modulate the electronic structure of the formed active sites. When used as a cathode catalyst, the constructed rechargeable zinc-air battery presents higher power density (268 mW cm −2 ), specific capacity (840 mAh g −1 ), and excellent stability. More importantly, the PtCo/NCNT catalyst allows the all-solid-state cell to exhibit remarkable flexibility and high round-trip efficiency at various bending states, demonstrating a potential possibility to replace the conventional Pt/C and RuO 2 catalysts.
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高影响因子
Nanoscale
·
2024
·Vol. 16
·期 26
·12492-12501
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IF 5.8
Zhichang Hu,Zhizhong Xiao,Wei Wei,Jian Yang,Xiaoyu Huang,Qingcheng Lu,Sundaram Chandrasekaran,Huidan Lu,Yongping Liu
The surface electronic structure and morphology of catalysts have a crucial impact on the electrocatalytic hydrogen evolution reaction performance. This work reports on the fabrication of a Ru-doped WP/WP2 heterojunction nanosheet array electrode via a one-step phosphating treatment of a Ru-doped WO3 precursor. Benefitting from the large electrochemical active surface of nanosheet arrays, rich WP/WP2 heterojunction interface, and trace Ru atom doping, the catalyst has a fairly low overpotential of 58.0 mV at 10 mA cm−2 and a Tafel slope of 50.71 mV dec−1 in acid solution toward the electrocatalytic HER. Further, theoretical calculations unveil that Ru atom doping and interface effect synergistically optimized the electronic structure of the catalyst and hence weakened the adsorption capacity of the catalyst surface toward hydrogen (H), which lowered the Gibbs free energy (ΔGH*) and consequently effectively improved the HER performance. This work may open new avenues for developing advanced nanoarray electrodes with efficient electrochemical energy conversion.
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Yirong Wang,Xuan Yu,Zhonghong Xia,Xuanrong Li,Ya Gao,Jing Zhang,Wuliang Feng,Xingli Zou,Yufeng Zhao
The high overpotential and sluggish kinetics of oxygen evolution reaction (OER) severely hinder the widespread application of electrochemical water splitting, especially at industrial-level current densities. Herein, we report a novel heterostructural Ni-based metal organic framework (MOF)-Ni 2 P in-situ grown on iron foam (NiMOF-Ni 2 P/IF), which shows remarkable OER activity and stability. We demonstrate that the work function difference between NiMOF and Ni 2 P leads to the strong electron coupling effect by promoting electron transfer at the interface and results in a discernible upward shift of the d-band center of Ni sites for favorable OH − adsorption. The as-fabricated NiMOF-Ni 2 P/IF exhibits an ultralow overpotential of 330 mV and a small cell voltage of 1.796 V to drive NiMOF-Ni 2 P/IF‖Pt/C system at 1000 mA cm −2 in 1 M KOH, outperforming the majority of state-of-the-art non-noble-metal-based electrocatalysts. Furthermore, the catalyst shows remarkable performance even under harsh industrial conditions of 40, 60, and 80 °C in 6 M KOH. In addition, NiMOF-Ni 2 P/IF holds great promise with remarkable stability of 200 h and 600 cycles in simulated seawater and secondary zinc-air batteries (ZABs), respectively. This work offers a rational design strategy for low cost, high activity, and long durability OER electrocatalyst based on in-depth comprehension of the electronic coupling effect.
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CHEMICAL ENGINEERING JOURNAL
·
2024
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IF 13.3
Qing-Qing Pang,Xi-Zheng Fan,Sha-Sha Yi,Xin Du,Zhong-Yi Liu,Xin-Zheng Yue
The design of bifunctional catalysts with spatially separated active sites holds significance importance in achieving simultaneous electrooxidation and hydrogen evolution reaction (HER). Herein, a core-shell Re-Ni@Ni(OH) 2 /CC heterostructure is demonstrated for the electrocatalytic furfural oxidation reaction (FOR) coupled with HER. Experimental results and theoretical analyses reveal that Re not only modulates the heterointerface between Re-Ni core and Ni(OH) 2 shell, facilitating furfural (FF) adsorption at Ni(OH) 2 sites, but also regulates electronic structure of Ni. This leads to a negative shift in the d-band center from Fermi level, effectively weakening hydrogen adsorption at Ni sites in Re-Ni@Ni(OH) 2 heterostructure, thereby improving the HER process. As a result, the synthesized Re-Ni@Ni(OH) 2 /CC exhibits a low cell voltage of 1.40 V @10 mA cm −2 for the FOR||HER. This study highlights the importance of modulating metal’s electronic structure and identifying active sites, which has great potential for improving bifunctional electrocatalytic reactions.
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ELECTROCHIMICA ACTA
·
2024
·
IF 5.5
Xuan Zheng,Yijun Liu,Zehua Zou,Qingxiang Wang
Developing efficient non-precious-metal-based bifunctional electrocatalysts for overall water splitting (OWS) is of great significance from both industrial and environmental perspectives. Herein, a novel flower-like architectured nanocomposite containing amorphous NiFe-hydroxide and NiFe-thiourea coordination complex, namely NiFe(O x H y )(TU)/NF, has been in situ synthesized on nickel foam by a simple simmer-assisted synthesis method. This nanomaterial demonstrates remarkable electrocatalytic performance and long-lasting durability for both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Specifically, the overpotentials required to achieve a current density of 50 mA cm −2 for HER and OER are as low as 273 and 243 mV, respectively. Moreover, the OWS electrolyzer assembled using NiFe(O x H y )(TU)/NF as both anodic and cathodic electrodes operates efficiently with an exceptionally low cell voltage of 1.47 V and 1.72 V at a current density of 10 mA cm −2 and 50 mA cm −2 , exhibiting negligible fluctuation over 55 hours. And this device can also be facilely driven by the photovoltaic cell. These excellent catalytic performances of NiFe(O x H y )(TU)/NF can be attributed to the electronic synergistic effects among multiple NiFe species like NiFe-hydroxide and NiFe-thiourea, as well as the abundant active sites induced by the nanoflower-like amorphous hierarchical structure. This study presents a practical and facile strategy for the synthesis of NiFe-based amorphous nanomaterial with robust OER and HER performances, thereby contributing to the advancement of multi-component bifunctional electrocatalysts.
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WATER RESEARCH
·
2025
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IF 12.4
Huanran Liu,Qinyan Yang,Chen Wang,Yang Wu,Li Liu,Guoqing Shen,Qincheng Chen
Microbial fuel cells (MFCs) offer great potential for simultaneous wastewater treatment and energy generation, yet the development of cost-effective and efficient carbon-based cathode alternatives to Pt/C for oxygen reduction reactions remains challenging. This study presents a novel single-atom Fe-decorated N-doped porous carbon (Fe-SA/NBC) synthesized from biogas residue for wastewater treatment. The Fe-SA/NBC demonstrated superior catalytic performance, achieving a kinetic current density of 18.89 mA·cm - ² compared to 10.38 mA·cm - ² for Pt/C, and an enhanced electrochemical surface area with a C dl of 1.81 mF·cm - ² versus 1.76 mF·cm - ² for Pt/C. When integrated into an MFC air-cathode under actual sewage, Fe-SA/NBC outperformed Pt/C, achieving a 22.6 % higher power density (882.92 mW·m - ² vs. 719.81 mW·m - ²), a higher output voltage (0.53 V vs. 0.47 V), and a longer operational duration (3.6 days vs. 3.2 days). Additionally, Fe-SA/NBC exhibited superior removal efficiencies for chemical oxygen demand and ammonia nitrogen during sewage treatment. In practical applications, MFCs equipped with Fe-SA/NBC successfully powered diodes and timers in series-connected configurations. This study introduces an innovative method for producing cost-effective and efficient cathode catalysts from waste biomass, offering significant potential for wastewater treatment and power generation systems.
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高影响因子
Surfaces and Interfaces
·
2025
·
IF 6.3
Tianping Wang,Yining Liang,Lin Xu,Xikui Liu,De Ning,Zhengjian Chen
Precisely modulating active sites to achieve high-performance catalysts remains a significant challenge but is critical to metal-air batteries and fuel cells. In this study, core-shell structured Co-TPG-IPOF/KB containing single cobalt (Co) atoms are anchored onto a 1,3,5-triformylphloroglucinol (TPG)- based ionic porous organic framework (IPOF) coated on Ketjenblack carbon (KB) was prepared through in-situ Schiff-base condensation. Systematic experimental characterizations reveal that KB cores provide abundant mesopores and greatly increase the accessible surface area from 48 to 614 m 2 g -1 , and the Co 2+ active sites are asymmetrically coordinated and uniformly dispersed upon the surface rather than inside the bulk. These remarkable structures enable Co-TPG-IPOF/KB to exhibit excellent oxygen reduction reaction (ORR) performance with a half-wave potential of 0.842 V, superior durability and methanol tolerance, and a favorable four-electron (4e - ) pathway, and therefore Zn-air batteries catalyzed by Co-TPG-IPOF/KB achieved considerably improved maximum power density (189 mW cm -2 ), specific capacity (727 mAh g zn -1 ), and cycling energy efficiency, superior to the benchmark Pt/C catalyst.
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ELECTROCHIMICA ACTA
·
2024
·
IF 5.5
Zhou Yang,Nan Jiang,Shaoyi Bei,Keyan Bao,Meng Xiang,Chengbin Yu,Shuang Dong,Hengfei Qin
Searching for an excellent bifunctional electrocatalyst used in zinc-air batteries (ZABs) is a long-term and challenging task. Single-atom catalysts have been becoming potential bifunctional electrocatalysts because of their maximum metal atom utilization and low content of metal itself. Herein, noble metal palladium (Pd) is uniformly anchored in the supported WO 2.72 to form single-atom Pd/WO 2.72 owing to the special 4d orbit of Pd and nonstoichiometric 2D planar structure of WO 2.72 . Single-atom 5 % Pd/WO 2.72 is prepared in this work, showing excellent bifunctional electrocatalytic behaviors with high E 1/2 of 0.86 V for ORR and low E j= 10 of 1.59 V for OER in alkaline medium, and the ∆E is 0.73 V, which outperforms the Pt/C and RuO 2 . Furthermore, the 5 % Pd/WO 2.72 -ZAB has a high open-circuit voltage (OCV) value of 1.491 V, a large power density of 168 mW cm −2 , and a large specific capacity of 633 mAh g −1 . Besides, the 5 % Pd/WO 2.72 -ZAB also has good cycling stability.
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