ACS Sustainable Chemistry & Engineering
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2022
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IF 9.224
Wenke Liu,Qingwei Qin,Hailin Zhang,Xing Chen,Ling Luo,Guangqiang Li,Shili Zheng,Ping Li
The conventional neutralization method for removing impurities Fe(III) and Al(III) from spent Li-ion battery (LIB) leaching solutions has encountered problems of low impurity removal efficiency or high loss of valuable metals. In this study, highly selective and effective separation of Fe(III) and Al(III) from spent LIB leaching solutions was achieved by the precipitation–complexation technology. It was found that almost all Fe(III) together with most of the Al(III) could be removed by preferential precipitation using NaHCO3 neutralization under an equilibrium pH of 3.3 at 95 °C. Phytic acid, as a selectively complexing agent, was then introduced to completely remove the residual Al(III) from Fe-removed solutions with an Al/PA molar ratio of 3:1 at 60 °C. As a result, more than 99.5% Fe(III) and 97.08% Al(III) could be removed from the actual solutions, with a total loss of Ni, Co, Mn, and Li of only 1.1%. Furthermore, the obtained Al-phytates could be decomposed to form Al(PO3)3 products at 1000 °C. The whole process not only realized the efficient removal of Al(III) and Fe(III) at low pH with minimal loss of Ni, Co, Mn, and Li but also reduced the emission of wastes and utilized the Al resources.
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ENVIRONMENTAL RESEARCH
·
2021
·
IF 6.498
Zhendong Yu,Jiachen Ma,Jinlan Dai,Shiyu He,Xiaoyi Huang,Yuancai Lv,Yifan Liu,Chunxiang Lin,Junfeng Chen,Minghua Liu
In this study, a bimetallic composite catalyst (Co–Fe@C) was fabricated with calcination at high temperature (800 °C) by using Co-MIL-101 (Fe) as the precursor. The characterization results showed that the resulted Co–Fe@C composite mainly consisted of carbon, FeCo alloys, Fe 3 O 4 , Co 3 O 4 and FeO, and owned evident magnetism. In addition, the Co–Fe@C was employed to activate the peroxydisulfate (PDS) to degrade a representative organic pollutant ( p -arsanilic acid, p -ASA) and the main factors were optimized, which involved 0.2 g L −1 of catalyst dosage, 1.0 g L −1 of PDS dosage and 5.0 of initial pH. Under the optimal condition, Co–Fe@C/PDS system could completely degrade p -ASA (20 mg L −1 ) in 5 min. In the Co–Fe@C/PDS system, SO 4 − · , Fe(IV) and ·OH were the main species during p -ASA degradation. Under the attack of these species, p -ASA was first decomposed into phenols and then transformed into the organics acids and finally mineralized into CO 2 and H 2 O through a series of reactions like hydroxylation, dearsenification, deamination and benzene ring opening. Importantly, most of the released inorganic arsenic species (93.40%) could be efficiently adsorbed by the catalyst.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
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IF 13.273
Kaibang Xiao,Fawen Liang,Jinzhi Liang,Weicheng Xu,Zhang Liu,Biru Chen,Xueding Jiang,Xiaolian Wu,Jianan Xu,Jingzi Beiyuan,Hailong Wang
Bimetallic Fe- and Ce-embedded N-enriched porous biochar (Fe-Ce@N-BC) was synthesized to activate peroxymonosulfate (PMS) for metronidazole (MNZ) removal. 97.5% decay of MNZ was achieved within 60 min in Fe-Ce@N-BC/PMS system. The kinetic reaction rate constant of the Fe-Ce@N-BC/PMS system (0.0566 min −1 ) was 10.5 times higher than that of the BC/PMS system (0.0054 min −1 ). The highly dispersed Fe-Ce oxide nanocrystals serve as PMS activation centers, while the addition of nitrogen source increases the surface area and porosity of biochar, as well as enhances the PMS activation performance. It is noteworthy that graphitic N and C O groups in biochar facilitates the PMS activation via a nonradical pathway and the Fe 2+ /Fe 3+ and Ce 3+ /Ce 4+ participate in the radical pathway. The presence of anion ions of SO 4 2− can promote the MNZ degradation process, while HCO 3 – and Cl − ions suppress the MNZ removal. The MNZ removal using Fe-Ce@N-BC in salty media behavior similarly with that in DDI water, while the decreased removal efficiency in real effluent could be mitigated by prolonging the reaction time. Finally, the degradation intermediate products of MNZ were identified and the pathway was proposed according to LC-MS analysis. The relatively low cytotoxicity of the Fe@Ce/N-BC evaluated by animal cell (A375) and toxicity evolution of MNZ intermediate products strongly suggest huge potential of utilization of the catalyst for aquatic environmental remediation.
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ACS Applied Materials & Interfaces
·
2021
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IF 9.229
Jiulong Wang,Weike Wang,Jianguo Li,Xueyang Mu,Xinyue Yan,Zerui Wang,Jinbu Su,Tao Lei,Chengbing Wang
Solar-driven interfacial steam generation (SDISG), as an emerging green and renewable approach to overcome water shortage, is very suitable for remote locations, developing countries, and disaster zones because it does not require an additional energy supply. However, the traditional metal-based and carbon-based absorbers always suffered from fragility (or rigidity) and the complex preparation process, which dramatically inhibited their transportation and installation in areas with poor infrastructure. Therefore, there is an urgent need to develop a universal method to fabricate flexible solar evaporators. Herein, a novel solar evaporator that integrates a flexible matrix (Cu mesh or textile) and a hierarchical Fe-MOF-74 photothermal absorber component is perfectly prepared for the rapid and efficient SDISG. Notably, the results show that Fe-MOF-74-based flexible textile matrix composites exhibit outstanding light absorption (83.81%), low thermal conductivity (0.1730 W/m K), super hydrophilic properties (within 50 ms, the contact angle is close to 0°), excellent salt resistance, high evaporation rate (1.35 kg/m2 h), and photothermal conversion efficiency (η is 81.5% under one sun, stable for 30 days). Owing to the flexibility, recyclability, and above-mentioned excellent performance, the prepared hierarchical Fe-MOF-74-based flexible composite systems are more practical for transportation, large-scale production, and stable and efficient applications. As a result, this work offers new insight into the future development of the combination of a MOF-based photothermal absorber and flexible substrates, as well as for the application of interfacial solar seawater desalination, and provides a new reference for other applications.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
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IF 13.273
Ran Yang,Qianqian Chang,Na Li,Hu Yang
Sulfate radical-based advanced oxidation processes have received increasing attention in contaminated water treatment. As an excellent electron donor, microscale zero-valent aluminum (mZVAl) is a promising persulfate (PS) activator. However, the natural oxide layer of mZVAl impedes electron transfer from the core metal. Herein, a composite comprising mZVAl and Fe-bearing clay (mZVAl-NaNAu-2) was obtained through the simple ball milling (BM), which synergistically activates PS for the efficient degradation of various organic contaminants, such as 4-chlorophenol, benzoic acid, nitrobenzene, phenol, and ofloxacin, in water. The sulfate radicals and hydroxyl radicals were the main reactive species but Fe(IV) was minor in this reaction. The BM can cause fracture of the mZVAl powder and promote exposure of the fresh Al 0 surface. Various Fe species in mZVAl-NaNAu-2 at different reaction times were evaluated by extraction experiments, Mössbauer and XPS spectra. Approximately 47.0% of structural Fe(III) was reduced to Fe(II) after BM. The dissolved Fe(II) and structural trioctahedral Fe(II)-Fe(II)-Fe(II) entities were mainly responsible for the homogeneous and heterogeneous activation of PS, and corroded mZVAl acted as an “electron pool” to regenerate the aforementioned Fe(II) species continuously. The mZVAl-NaNAu-2/PS system also presented certain resistance to a natural organic matter and some anions, such as Cl - and NO 3 - . This study provided a new strategy for the efficient removal of organic contaminants from water and also solved the bottleneck of mZVAl in applications due to its dense oxide film.
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高影响因子
ACS Omega
·
2021
·
IF 3.512
Chang Xu,Wenlu Yang,Jiaxin Zhao,Jingyuan Ma,Mingxing Wu
In the present study, three types of specific solid, core–shell, and hollow structured cobalt and iron co-doped MoS2 nanocubes (denoted as s-Co-Fe-MoSx, c-Co-Fe-MoSx, and h-Co-Fe-MoSx) are controllably synthesized for the first time by regulating the reactant mass ratios. The prepared Co-Fe-MoSx nanocubes can function as a counter electrode in dye-sensitized and perovskite solar cells (DSCs and PSCs) and a working electrode in a supercapacitor. In the DSC system, the c-Co-Fe-MoSx nanocubes exhibit the maximum catalytic activity to the Co3+/2+ redox couple regeneration, and the device achieves a power conversion efficiency (PCE) of 8.69%, significantly higher than the devices using s-Co-Fe-MoSx (6.61%) and h-Co-Fe-MoSx (7.63%) counter electrodes. Similarly, all of the prepared Co-Fe-MoSx nanocubes show decent activity in PSCs and the device using the c-Co-Fe-MoSx counter electrode achieves the highest PCE of 6.88%. It is worth noting that, as the supercapacitor working electrode, the h-Co-Fe-MoSx exhibits a specific capacitance of 85.4 F g–1, significantly higher than the parallel values achieved by the s-Co-Fe-MoSx and c-Co-Fe-MoSx electrodes under identical conditions.
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ACS Applied Materials & Interfaces
·
2021
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IF 9.229
Guang Li,Juan Yang,Yulian Chen,Min Liu,Xiaowei Guo,Gairong Chen,Baobao Chang,Tianjing Wu,Xianyou Wang
Looking for a high-efficiency, durabile, and low-cost dual-functional oxygen electrocatalyst as the air electrode catalyst in rechargeable zinc-air batteries (ZABs) is urgently desirable but faces many challenges. Herein, we propose the preparation strategy of effectively using a bifunctional electrocatalyst (Fe–Nx/C) based on the zeolite imidazole organic framework-8 (ZIF-8) as the template agent, with surface modification coated by ferrocene (Fc) molecules followed by pyrolysis at high temperature under inert atmosphere. Benefiting from the surface modification of ZIF-8 with Fc molecules, more abundant multiple catalytic Fe/Fe–Nx/FeCx sites with high intrinsic activity are derived, the resultant Fe–Nx/C exhibits excellent potential gap (ΔE = 0.63 V) and durability, which is obviously superior to the Pt/C + IrO2 benchmark (ΔE = 0.77 V) and other state-of-the-art electrocatalysts. Furthermore, the assembled rechargeable ZABs employing the Fe–Nx/C as an air-electrode show a reduced charging–discharging potential difference of 0.603 V, high power density of 214.8 mW cm–2, and long-term cycling stability of more than 290 h at 2.0 mA cm–2. Therefore, this work presents a feasible strategy to prepare a high-efficiency and durability ORR/OER bifunctional electrocatalyst toward high performance ZABs and next-generation energy storage devices.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
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IF 5.816
Jiaxian Liu,Guyang Ning,Kun Shi,Man Zheng,Yuena Sun,Yongjun Gao,Yufan Zhang,Huan Wang
In this work, a string of different proportion trimetallic loaded the N-doped hollow porous carbon nanospheres (N-HPCS@Co Cu Fe NSs) were successfully crafted by a simple and economical method. Herein, the hollow-carbon structure was formed by etching carbon nanospheres. Moreover, owing to the presence of the PDA and P123, high dispersed nano spheres with mesopores were obtained. By this way, the catalyst can expose unique internal cavity and short transport path. Meanwhile, trimetal-based metal-organic frameworks (MOFs) Co Cu Fe alloy nano spheres (Co Cu Fe NSs) are first prepared. Creatively, PDA acts as the carbon resource, nitrogen resource and metal grafting agent simultaneously. Through a series of tests, N-HPCS@Co 1 Cu 1 Fe NSs has the best electrocatalytic performance and durable stability. This work highlights the current advances of hollow porous carbon structure, trimetallic active sites and N-doping, as well as, endow high electrocatalytic activity and durability for HER and OER .
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RSC Advances
·
2021
·Vol. 11
·期 43
·26502-26508
·
IF 3.361
Meirong Fu,Mingqiang Li,Yingying Zhao,Yunxiang Bai,Xingzhong Fang,Xiaolong Kang,Min Yang,Yanping Wei,Xia Xu
Precious metal nanometric catalysts are widely used in the removal of harmful substances. In the process of synthesis and catalytic reaction, it is particularly important to study green and simple synthesis methods and high catalytic efficiency. In this paper, a green one-step method was used to synthesize the Fe(OH)3/Fe2O3@Au composite catalyst, in which Au was single atom-dispersed. The removal of 4-nitrophenol (4-NP), a typical dangerous chemical widely existing in factory waste gas, waste water and automobile exhaust gas, was catalysed by Fe(OH)3/Fe2O3@Au. The catalytic performance of Fe(OH)3/Fe2O3@Au with different synthesis conditions (different amounts of MES, NaBH4, FeSO4, Au and Pt) on the 4-NP reduction reaction were systematically studied. Finally, the stability and recyclability of Fe(OH)3/Fe2O3@Au composite nanocatalyst were investigated thoroughly.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
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IF 7.312
Chan Zhou,Lei Zhu,Lin Deng,Haojie Zhang,Hanxuan Zeng,Zhou Shi
For improving the catalytic activity and recyclability of CuS in Fenton-like reaction processes, novel sulfur vacancies-enriched CuS@MIL-101(Fe) was constructed, characterized, and examined as heterogeneous catalysts for activating peroxymonosulfate (PMS) to degrade coumarin (COU). Thanks to the redox pairs of Fe 3+ /Fe 2+ , Cu + /Cu 2+ , S 2− /S 2 2− /S 0 /sulfate species, copper-iron synergistic effect and sulfur vacancies, the CuS@MIL-101(Fe) realized a complete removal of COU (30 μM) in 10 min with reaction rate constant of 0.577 min −1 , which was 11.1 and 17.0 times of CuS and MIL-101(Fe), respectively. The effect of various experimental conditions (i.e., initial pH, CuS@MIL-101(Fe) dosage, PMS concentration, and background anions) on COU degradation was discussed, and the stability and versatility of CuS@MIL-101(Fe) was studied as well. Radical scavenging experiments and electron paramagnetic resonance (EPR) spectroscopy identified • OH and 1 O 2 as the main reactive oxygen species (ROS). Finally, the possible mechanism of higher COU degradation efficiency in the CuS@MIL-101(Fe) activated PMS system and the degradation pathways were also deeply explored. Consequently, this work provided a novel insight into construction of sulfur vacancies-enriched heterogeneous catalysts for efficiently activating PMS for refractory organic pollutants elimination.
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高影响因子
CHEMOSPHERE
·
2021
·
IF 7.086
Yu Cao,Shanqing Jiang,Xudong Kang,Hankun Zhang,Qiuya Zhang,Liping Wang
In this study, Fe-phenol modified biochar was prepared to enhance atrazine (AT) degradation by ferrate (Fe(VI)) under alkaline conditions, and the properties, mechanism and transformation pathways were extensively investigated. Degradation experiments showed that Fe-phenol modified biochar was more beneficial for improving the oxidation capacity of Fe(VI) than unmodified biochar, and the biochar with a molar ratio of Fe 3+ to phenol of 0.1:5 (BC-2) showed the best promoting effect, and more than 94% of AT was removed at pH = 8 within 30 min. Moreover, the rate of oxidation ( k app ) of AT by Fe(VI) increased 1.86 to 4.11 times by the addition of BC-2 in the studied pH range. Fe(Ⅴ)/Fe(Ⅳ) and ·OH were the main active oxidizing species for AT degradation in the Fe(VI)/BC-2 group and contributed to 70% and 24%, respectively, of degradation. The formation of ·OH and Fe(Ⅴ)/Fe(Ⅳ) was mainly due to the persistent free radicals and reducing groups on the surface of BC-2. AT was oxidized to 12 intermediate products in the Fe(VI)/BC-2 group through 5 pathways: alkyl hydroxylation, dealkylation, dichlorination, hydroxylation, alkyl dehydrogenation and dichlorination. Compared with those of the initial solution, the total organic carbon content and toxicity after the reaction decreased by 32.8% and 19.02%, respectively. Therefore, the combination of Fe-phenol modified biochar and Fe(VI) could be a promising method for AT removal.
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2021
·Vol. 45
·期 14
·6424-6431
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IF 3.591
Jingjing Ju,Jiajia Lu,Xiaoyue Shi,Hongwei Zhu,Han-Pu Liang
Exploring efficient electrocatalysts with low production costs for the oxygen evolution reaction (OER) is significant for sustainable and scalable production of hydrogen through water electrolysis, while it still remains a challenge. Herein, mesoporous Fe-doped Co–Ni oxide (CoNiFeOx) nanosheets grown on nickel foam are synthesized by a facile two-step strategy (a combination of hydrothermal and post-annealing). Benefiting from the mesoporous nanosheet structure, endowing the catalysts with a high specific surface area (222.6 m2 g−1) and more active sites, and the optimized electronic structure due to the incorporation of Fe, the as-synthesized mesoporous CoNiFeOx nanosheets as a binder-free electrode exhibits remarkable OER activity with an overpotential of only 221 mV at a current density of 10 mA cm−2 and a small Tafel slope of 43.8 mV dec−1 in 1 M KOH solution. Besides, it displays excellent stability for over 250 h and no obvious activity decline is measured after the long-term stability test. Our strategy will provide a potential route to develop low-cost and high-performance electrocatalysts for the OER.
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