Nature Communications
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2024
·Vol. 15
·期 1
·1-12
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IF 14.7
Cai Zhengwei,Liang Jie,Li Zixiao,Yan Tingyu,Yang Chaoxin,Sun Shengjun,Yue Meng,Liu Xuwei,Xie Ting,Wang Yan,Li Tingshuai,Luo Yongsong,Zheng Dongdong,Liu Qian,Zhao Jingxiang,Sun Xuping,Tang Bo
Electrocatalytic H 2 production from seawater, recognized as a promising technology utilizing offshore renewables, faces challenges from chloride-induced reactions and corrosion. Here, We introduce a catalytic surface where OH – dominates over Cl – in adsorption and activation, which is crucial for O 2 production. Our NiFe-based anode, enhanced by nearby Cr sites, achieves low overpotentials and selective alkaline seawater oxidation. It outperforms the RuO 2 counterpart in terms of lifespan in scaled-up stacks, maintaining stability for over 2500 h in three-electrode tests. Ex situ / in situ analyses reveal that Cr(III) sites enrich OH – , while Cl – is repelled by Cr(VI) sites, both of which are well-dispersed and close to NiFe, enhancing charge transfer and overall electrode performance. Such multiple effects fundamentally boost the activity, selectively, and chemical stability of the NiFe-based electrode. This development marks a significant advance in creating durable, noble-metal-free electrodes for alkaline seawater electrolysis, highlighting the importance of well-distributed catalytic sites.
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Journal of Cleaner Production
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2024
·
IF 9.7
Jiaqun Zou,Bingen Yuan,Chuanxi Zhao,Jianxin Wang,Haoqi Qiu,Jiaxin Dang,Qin Wang,He Miao,Jinliang Yuan
Cobalt (Co) is widely used in energy storage and conversion devices, although its content on our planet is not adequate. Therefore, recycling Co from the spent Co-enriched materials is indispensable. Co-based perovskites , which contain abundant Co, are extensively utilized in solid oxide fuel cells, three-way catalysts, and oxygen-permeable membranes, and the recovery of Co from the spent Co-based perovskites is necessary to meet the long-term requirement of Co. In this work, a facile and universal thermal reduction method (750 °C and N 2 atmosphere) is employed to convert the spent cobalt-based perovskites into high-performance bifunctional oxygen catalysts for zinc-air batteries (ZABs), achieving high-efficient Co recovery and re-utilization. At high temperatures, melamine and dopamine hydrochloride are transformed into carbon nanotubes , C 3 N 4 and reducing gases (such as NH 3 and H 2 ). Simultaneously, the metal elements in the spent Co-based perovskites (SrNb 0.1 Co 0.7 Fe 0.2 O 3 ,SNCF) are converted into nano-scale alloy particles and metal nitrides . Then, the phase structures, micromorphology, and element valences of the obtained multiphase oxygen catalyst (SNCF–Ni-PM) are characterized by X-ray diffraction, scanning/transmission electron microscopy, and X-ray photoelectron spectroscopy, respectively. The electrochemical properties , including oxygen catalytic activities and stability, of SNCF-Ni-PM are measured by linear sweep voltammetry , chronopotentiometry, chronoamperometry, and cyclic voltammetry methods. Considering the practical applications, the aqueous and solid-state ZABs are assembled and measured. The results demonstrate that the multiphase SNCF-Ni-PM mainly includes carbon nanotubes, C 3 N 4 nanosheets , and FeNiN or CoFe nanoparticles . Moreover, SNCF-Ni-PM exhibits excellent bifunctional oxygen catalytic activity, with an oxygen evolution reaction (OER) potential at 10 mA cm −2 of 1.51 V and an oxygen reduction reaction (ORR) half-wave potential of 0.77 V, outperforming most of the reported oxygen catalysts. Using SNCF-Ni-PM, the aqueous and solid-state ZABs can achieve high power densities of 295.9 and 228.4 mW cm −2 , respectively, being superior to most ZABs. In addition, the aqueous ZAB with SNCF-Ni-PM can operate stably for 300 h with a slight degradation. This work provides a feasible method for effectively recycling Co from the spent Co-based perovskites.
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GREEN CHEMISTRY
·
2024
·Vol. 26
·期 13
·8020-8029
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IF 9.3
Jianglin Liu,Xueqing Qiu,Shirong Sun,Bowen Liu,Yuhui Tian,Yanlin Qin,Xuliang Lin
The utilization of plant polyphenols as catalyst carriers holds promise for environmentally friendly catalysis. However, challenges such as the inhomogeneous distribution of organic ligands often hinder their effectiveness. In this study, lignin–metal supramolecular framework were formed through ionic coordination self-assembly, achieved by oxidative ammonolysis modified lignin. The specific spatial domain-limiting effect of lignin–metal supramolecular framework ensures the dispersion and stability of catalyst active sites. Carbon-coated trimetallic catalysts (Ru–FeNi@OALC) derived from lignin–metal supramolecules exhibit promising performance, with low overpotentials for the oxygen evolution reaction (OER, η10 = 290 mV) and the hydrogen evolution reaction (HER, η10 = 52 mV), surpassing commercial noble metal catalysts. Additionally, these catalysts demonstrate long-lasting water-splitting performance, highlighting their potential for sustainable catalytic reactions. Molecular simulations and DFT theoretical calculations elucidate the feasibility of lignin oxidative ammonolysis modification and reveal the coordination mechanism. Furthermore, the abundant defects and disorder in the coordination polymer-derived carbon materials optimize electron transfer processes and accelerate reaction kinetics. This construction strategy towards designable polyphenol–metal supramolecular framework presents a promising avenue for the green synthesis of a variety of metal/carbon composite catalysts, contributing to sustainable catalysis and environmental protection.
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Feng Feng,Jiaying Zhang,Lu Yu,Haixin Wang,Heda Ding,Jifan Cheng,Miaolan Wang,Fangfang Chen,Jiahui Zhang,Lingling Guo,Chunshan Lu,Qunfeng Zhang,Xiaonian Li
In order to develop an efficient and environmentally friendly method for the recovery of precious metals, a functionalized ionic liquid containing free radicals (1-methyl-3-(2-oxo-2-(2,2,6,6-tetramethyl-1-oxo-4-piperidinoxy) butyl) imidazole trichloro-1-bromoaluminium salt) was designed and synthesized. This was achieved by combining 2,2,6,6-tetramethylpiperidine-1-oxyl (TEMPO), which possesses oxidizing properties, with halide ions that exhibit complexing abilities. Notably, under optimal conditions, a maximum gold dissolution rate of 100 % was attained. X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), and Raman spectroscopy analyses were conducted to elucidate the dissolution mechanism. Ultimately, these functionalized ionic liquids can be utilized for the dissolution of precious metals in CPU pins and waste catalysts. This study presents an effective approach for the recovery of precious metals.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
·
IF 9.4
Wenxin Wang,Jiangjiang Zhang,Jinsheng Rong,Lanli Chen,Shiqiang Cui
Reducing the size of catalysts and tuning their electronic structure and interfacial properties are key to enhancing catalytic performance. Herein, a series of quantum-sized Co-based nanodot composites, including Co 3 O 4 /C, CoS 2 /C, CoN/C, and CoP/C, were synthesized using chemical vapor deposition (CVD) methods. By means of experimental measurement and theoretical calculation, CoP/C exhibited more robust electrochemical response than other Co-based compounds in electrochemical oxidation of N 2 H 4 (HzOR) and hydrogen evolution reaction (HER). The catalytic activities of CoP/C can be further enhanced by introducing Co vacancies on the surface of CoP/C (labeled as Co 1−x P/C). The results demonstrated that Co 1−x P/C not only exhibited notable electrochemical responses at an ultra-low N 2 H 4 concentration of 0.67 μM, showcasing its potential for ultra-sensitive N 2 H 4 detection but also realized HzOR instead of the oxygen evolution reaction (OER) half-reaction, thereby lowering the overpotential to 2.0 mV at 10.0 mA cm −2 . Finally, a Zn-hydrazine (Zn-Hz) battery was fabricated as a promising energy conversion device, showing the exceptional practical value of Co 1−x P/C.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Zhuang Wang,Mian Li,Bin Fu,Wenping Cao,Xiangjie Bo
Although cobalt nitride (CoN)-based nanomaterials have been widely designed as advanced oxygen evolution reaction (OER), hydrogen evolution reaction (HER), and oxygen reduction reaction (ORR) catalysts, the continuous consumption of lithium-ion batteries (LIBs) has led to a high price of cobalt metal. Therefore, in the future, recycling valuable Co elements from spent devices and boosting their service efficiency will inevitably promote the utilization of Co-based materials in water splitting and zinc-air batteries (ZABs). Herein, we realize the Co recycling from spent LIBs by a simple hydrometallurgy method. Under the assistance of hexamethylenetetramine and polystyrene spheres, after the hydrothermal and pyrolysis treatment in the NH 3 atmosphere, the as-reclaimed cobalt oxalates were successfully transformed into novel three-dimensional (3D) CoN nanoflowers (denoted as CoN NFs). Benefiting from the unique 3D flower-like architectures, intrinsic high conductivity, large surface area, uniformly dispersed CoN nanoparticles, and the synergistic effect between Co 3 N and CoO phases, the 3D flower-like CoN NFs exhibited excellent OER catalytic activity. The performance was much better than commercial RuO 2 in the 1.0 M KOH solution. Furthermore, the CoN NFs-based water splitting cell needed a voltage of 1.608 V to achieve the current density of 10 mA cm −2 , which is even 16 mV smaller than that of Pt/C||RuO 2 benchmark (1.624 V). Meanwhile, the CoN NFs-derived ZAB exhibited a high peak power density of 107.3 mW cm −2 (vs. 103.2 mW cm −2 of Pt/C-RuO 2 -based ZAB) and a low charge–discharge voltage gap (0.93 V vs. 1.43 V of Pt/C-RuO 2 -based ZAB). Due to the excellent structural and elemental stabilities, the corresponding water splitting cell and ZAB had outstanding durability. This work successfully explored an advanced industrial chain from recycling Co metal in spent devices to designing the high-efficiency HER/OER/ORR electrocatalysts for advanced water splitting devices and ZABs. This will further promote the value-added utilization of valuable Co metal in various energy storage or conversion devices.
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ACS Applied Nano Materials
·
2024
·
IF 5.3
Zhuang Wang,Mian Li,Wenping Cao,Xiangjie Bo
Enhancing catalytic efficiency, achieving controlled synthesis, and lowering production costs are crucial for promoting the use of cobalt oxide (CoOx)/cobalt nitride (CoNx) composites in full water splitting and electrochemical sensing. In this study, a three-dimensional (3D) hierarchically porous material composed of numerous two-dimensional (2D) porous CoOx/CoNx nanosheets (denoted as CoOx/CoNx NSs) was synthesized by using cobalt oxalates (COs) recycled from spent lithium-ion batteries. In a 1.0 M KOH solution, the 2D porous CoOx/CoNx NSs exhibited higher oxygen evolution reaction (OER) electrocatalytic activity than commercial ruthenium oxide (RuO2). Meanwhile, the CoOx/CoNx NSs exhibited a slightly lower hydrogen evolution reaction (HER) electrocatalytic activity than 20 wt % platinum/carbon (Pt/C). Moreover, the CoOx/CoNx NS-based full water-splitting electrolyzer achieved a current density of 10 mA cm–2 at 1.562 V, which was 49 mV more positive than the 1.489 V of the Pt/C||RuO2 benchmark. Furthermore, the 2D porous CoOx/CoNx NSs featured significantly higher HER, OER, and full water-splitting catalytic stability than Pt/C/RuO2. Moreover, the CoOx/CoNx NS-based nonenzymatic electrochemical sensor exhibited advanced glucose detection performance. Particularly, the sensor had a wide linear range of 1.0–10.5 mM), a low detection limit of 5.0 μM), and a fast response time of 0.6 s. The 2D porous CoOx/CoNx NSs exhibited excellent catalytic activity owing to their 3D hierarchically porous architectures, large surface area, good conductivity, uniformly dispersed active sites, and synergistic effects of CoNx and CoO. This study presents an advanced model for recycling Co metal from spent devices and designing advanced Co-based electrocatalysts for water splitting and electrochemical sensing.
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GREEN CHEMISTRY
·
2024
·
IF 9.3
Shumin Huang,Xiaolin Luo,Ji Li,Sibao Liu,Li Shuai
High-density fuel additives are important for heavy transportation. Production of high-density fuel additives from renewable resources has been receiving increasing attention in recent years. Despite the progress in the depolymerization of lignin, cellulose, and hemicelluloses, there are limited studies on integrating lignin and carbohydrates to make value-added products. Here we design a route to synthesize high-density fuel additives with lignin-derived monophenolics and carbohydrate-derived furanics. We performed Brønsted base-catalyzed C–C coupling of phenolics and furanics followed by hydrodeoxygenation catalyzed by a synthesized Ir–ReOx/SiO2 catalyst. Under optimized reaction conditions, the coupling product of phenolics and furanics, bicyclic furyl phenyl precursors, reached a yield of over 90%, and was further hydrodeoxygenated to bicyclohexyl alkanes with a yield of over 98%. The current two-step strategy demonstrates high-selectivity of preparing high-density hydrocarbon fuels from lignocelluloses and provides a possible way to utilize all components of lignocellulosic biomass in an integrated upgrading pathway.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
·
IF 8.1
Zhenzhong Liu,Suyue Luo,Xinran Yin,Shuo Zhang,Minghui Guo
The present work effectively achieved the production of a self-supporting electrode with high efficiency. The process involves incorporating nickel and molybdenum carbide (Mo 2 C) phases within the channels of wood through high-temperature calcination at the nanoscale. The obtained carbonized wood (CW) possesses low tortuosity and three-dimensional vertical channels, providing an excellent substrate for the preparation of Ni-Mo 2 C/N-CW electrodes. Mo 2 C is well known for its considerable potential as a non-precious metal electrocatalyst with enhanced catalytic activity. The successful doping of nickel and nitrogen into molybdenum carbide not only promotes the formation of β-Mo 2 C, but also improves the electron transfer rate and mass diffusion pathway. Consequently, the Ni-Mo 2 C/N-CW electrode exhibits excellent performance in the hydrogen and oxygen evolution reactions (HER and OER, respectively). Only voltages of 89 and 253 mV are required to achieve a current density of 10 mA cm −2 , respectively. When the Ni-Mo 2 C/N-CW catalyst is used as both cathode and anode during hydrolysis, current densities of 10 and 100 mA cm −2 can be achieved with excellent durability and stability at voltages of 1.56 and 1.72 V, respectively. The distinctive porous structure of the wood substrate is of crucial importance for promoting the adsorption and dissociation of water molecules, enhancing the catalytic performance. In addition, the present material exhibits advantageous characteristics, including a high specific surface area and a significant number of adsorption sites, making it a very promising candidate for applications involving the adsorption of dyes, such as rhodamine B (RhB).
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Lixia Wang,Jia Huang,Xinran Hu,Zhiyang Huang,Mingcheng Gao,Di Yao,Tayirjan Taylor Isimjan,Xiulin Yang
The pursuit of efficient and economically viable catalysts for liquid/solid-state zinc-air batteries (ZABs) is of paramount importance yet presents formidable challenge. Herein, we synthesized a vacancy-rich cobalt/manganese oxide catalyst (Co/MnO@NC) stabilized on a nitrogen-doped mesoporous carbon (NC) nanosphere matrix by leveraging hydrothermal and high-temperature pyrolysis strategy. The optimized Co/MnO@NC demonstrates fast reaction kinetics and large limiting current densities comparable to commercial Pt/C in alkaline electrolyte for oxygen reduction reaction (ORR). Moreover, the Co/MnO@NC serves as an incredible cathode material for both liquid and flexible solid-state ZABs, delivering impressive peak power densities of 217.7 and 63.3 mW cm −2 and robust long-term stability (459 h), outperforming the state-of-the-art Pt/C and majority of the currently reported catalysts. Research indicates that the superior performance of the Co/MnO@NC catalyst primarily stems from the synergy between the heightened electrical conductivity of metallic Co and the regulatory capacity of MnO on adsorbed oxygen intermediates. In addition, the abundance of vacancies regulates the electronic configuration, and superhydrophilicity facilitates efficient electrolyte diffusion, thereby effectively ensuring optimal contact between the active site and reactants. Besides, the coexisting NC layer avoids the shedding of active sites, resulting in high stability. This work provides a viable approach for designing and advancing high-performance liquid/solid-state ZABs, highlighting the great potential of energy storage technology.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Huamei Tong,Xinyu Zheng,Mengyue Qi,Di Li,Jianjun Zhu,Deli Jiang
Constructing bifunctional non-precious metal electrocatalysts with advanced industrial value and excellent electrocatalytic performance to achieve efficient overall water splitting is important but difficult. Herein, a heterogeneous electrocatalyst comprising of CoMo alloys anchored Fe 2 O 3 nanosheets was prepared by hydrothermal and electrodeposition methods. The strongly coupled interfaces between the CoMo alloys and Fe 2 O 3 nanosheets promote charge redistribution, which could improve electron transfer efficiency and accelerate reaction kinetics, potentially optimizing reactant adsorption energy. Further density functional theory (DFT) calculations reveal that the construction of CoMo/Fe 2 O 3 /NF heterostructured catalyst facilitates to promote interfacial charge redistribution and enhance charge transfer capacity, thus boosting the catalytic performance. Benefiting from this, the optimal CoMo/Fe 2 O 3 /NF heterostructure demonstrates a minimal overpotential of 71 mV at 10 mA cm −2 for the HER and 266 mV at 50 mA cm −2 for the OER. Remarkably, the catalyst served as a bifunctional electrode for water splitting, resulting in a cell voltage down to 1.5 V at a current density of 10 mA cm −2 . This research provides an effective way for the construction of non-precious iron oxides-based bifunctional electrocatalysts using alloy/metal oxide interfacial engineering strategy.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Yang Liu,Hailong Feng,Weiyi Li,Xueping Wang,Guoxiang Huang,Longxia Wang,Xingqiu Li,Yuxing Xie,Chenglu Liang
Catalysts in-situ reconstructed from transition metal sulfides for oxygen evolution reaction (OER) have been regarded as potential alternatives for the noble metal catalysts . Intriguingly, it was found that the self-optimized SO 4 2− @Cu doped Co(OH) 2 catalyst was reconstructed from bimetallic sulfide of CuCo 2 S 4 . During the OER process, the copper was partially leached and meantime doped into the in-situ generated Co(OH) 2 with SO 4 2− adsorption, while only oxides were discovered in counterparts of mono-metal sulfides. As a result, the SO 4 2− @Cu doped Co(OH) 2 catalyst exhibited superior OER performances, with low overpotentials of 211/272 mV to achieve the current densities of 10/100 mA cm −2 , exceeding the counterparts reconstructed from mono-metal sulfides. Experimental and theoretical results suggested that the in situ generated Cu doped Co(OH) 2 possessed thin and loosely layered structure with expanded lattice spacing (lattice spacing expanded from 0.28 nm to 0.46 nm) due to the SO 4 2− adsorption, making the intermediates more accessible to the active centers. In addition, the catalyst surface changed from hydrophobicity to super hydrophilicity , which greatly accelerated the mass transfer. This work indicated that the in-situ reconstruction process was greatly influenced by the interactions between metal sites and sulfide species, directly influencing the OER performances of the reconstructed catalysts.
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