CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Wenxuan Zhou,Xiaoyong Mo,Cham Wah Cheung,Edmund C.M. Tse
At present, over 95 % of H 2 O 2 is produced via the anthraquinone process that requires large infrastructure, generates organic pollution, and poses safety issues. Electrochemical H 2 O 2 generation through oxygen reduction can serve as an alternative, reliable, and decentralized production method if affordable and high-performance electrocatalysts can be developed. Herein, a two-step process is used to prepare an Fe-based complex as a non-precious metal electrocatalyst to facilitate oxygen reduction reaction (ORR) and produce an alkaline H 2 O 2 solution. The Fe complex of benzene-1,3,5-tricarboxylate (FeBTC) is first synthesized using a hydrothermal method and then activated via a pulsed laser treatment process that is optimized via the Taguchi method. The pulse-laser-treated FeBTC (PL-FeBTC) lowers the H 2 O 2 electrosynthesis overpotential by 50 mV at −0.1 mA/cm 2 and exhibits a 25 % increase in H 2 O 2 product selectivity at 0.4 V vs. RHE. The experimental results indicate that the O 2 -to-H 2 O 2 turnover frequency and electrocatalytic yield of the Fe-based metal–organic framework are enhanced simultaneously through solid-to-solid pulsed laser conversion. Through a series of X-ray photoelectron spectroscopy, elemental analysis, Raman spectroscopy, X-ray absorption spectroscopy, and control atmospheric experiments, the origin of the improvement in catalytic performance is rationalized through the formation of an oxo-bridge across the di–Fe active site via an oxygen-doping mechanism, thus providing a systematic laser methodology for precise structure-performance tuning. Beyond H 2 O 2 generation, this study further lays the foundation for the development of cost-effective and scalable electrocatalysts that are central to other commodity manufacturing and sustainable resourcification processes.
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DOI
高影响因子
FUEL
·
2025
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IF 7.5
Xiaodan Zhang,Yongjun Zhang,Hongjing Han,Yanan Zhang,Haiying Wang,Jiayu Zhang,Xinyu Liu,Yanguang Chen
Great progress has been made in the catalytic cracking of shale oil by introducing metals into zeolites for regulating acidity to tailor the distribution of olefin products. However, the interaction between the loaded bimetals and their synergistic effect with the acid sites of the zeolite remains controversial. In this work, catalysts of highly stable Fe-La bimetals confined in ZSM-35 zeolite (Fe-La-ZSM-35) were constructed with appropriate acidic properties. Real shale oil and n -heptane as a representative reactant were chosen to explore the catalytic cracking performance of these materials. The Fe-La species formed metal sites bonded to the zeolitic framework in the confined microenvironment of ZSM-35, which established strong interactions. Comparing Fe-La-ZSM-35 with Fe/La-ZSM-35 synthesized by the impregnation method revealed that the direct doping method could better incorporate La and Fe species within the zeolite, resulting in stronger interactions between the bimetals and framework aluminum to form a large number of medium-strong Lewis acid sites (Fe-OH). The ratio of Brønsted acid sites to Lewis acid sites decreased from 1.56 in Fe/La-ZSM-35 to 0.45 in Fe-La-ZSM-35. Furthermore, the electron cloud density at the active Fe-OH site increased due to electron transfer from La to Fe, which promoted the adsorption of carbocations, improved stabilisation of carbocations and bimolecular reactions were inhibited. And the C 3 -C 4 bonds of n -heptane molecules were more easily attacked due to the weak acidity of these acid sites, resulting in propylene being the main product as the reaction C 7 H 16 → C 4 H 10 + C 3 H 6 was dominant during the catalytic cracking of n -heptane. The propylene yield of Fe-La-ZSM-35 increased to 35.35% compared with La-ZSM-35 (22.62%) and Fe/La-ZSM-35 (26.16%) at 600°C. During three reaction-regeneration cycles, n -heptane conversion and propylene selectivity were as high as 89.33% and 30.85%. For real light shale oil, the catalyst achieved a propylene yield and selectivity of 19.24% and 31.0%, demonstrating excellent feedstock generalizability. In addition, Fe-La-ZSM-35 exhibited excellent stability, indicating considerable potential for use in the catalytic cracking of real oil.
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2025
·
IF 2.5
Sleshi Fentie Tadesse,Worku Lakew Kebede,Dong-Hau Kuo
Visible-light-driven photocatalysis is an efficient and environmentally benign approach to mitigate organic pollutants from waste effluents. A facile one-step precipitation method was used to synthesize Fe–Mo3(O,S)4−x/La4Mo2O11 (FeLaMoOS) nanocomposites. The as-prepared materials were characterized by XRD, SEM, HR-TEM, XPS, PL, EIS, photocurrent, and UV-visible spectroscopy. The type I heterojunction formed between Fe–Mo3(O,S)4−x and La4Mo2O11 exhibited a maximum light absorption response in the visible spectrum. The FeLaMoOS composite (13% Fe and 20% La) demonstrated the highest degradation efficiency, degrading 97.5% MO and 99.2% RhB in 90 min. The removal efficiency of MB was 99.6% after 45 min of magnetic stirring in the dark. The enhanced catalytic efficiency can be attributed to the effective charge separation of photoinduced e−–h+ pairs due to doping and heterojunction formation. Superoxide radicals (O2˙−) played a dominant role, while hydroxyl radicals (˙OH) played only a minor role, in the photocatalytic degradation process. Possible photocatalytic degradation mechanisms of organic dye molecules were proposed, based on the active radical species involved and the band potentials of the photocatalysts. This study can be used to establish a simple and efficient strategy for designing reusable composite photocatalysts for the degradation of organic dyes.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Yanhua Xie,Mingyue Hu,Jiahao He,Haiyan Hu,Tianliang Zheng,Silu Lv,Shengyan Pu
Alkaline As(III)-contaminated wastewater, which is prevalent at tunnel-construction sites, poses a serious risk to the environment and human health. However, the existing research on the treatment of this alkaline wastewater is scarce. Herein, we proposed a treatment method based on a Fe(II)/CaSO 3 system enhanced by highly alkaline As(III)-contaminated wastewater (pH: ~12) itself. Mechanistic investigations revealed that alkaline conditions enhanced the process in two ways: (i) by accelerating the Fe(II)/Fe(III) cycle to sustain · OH and SO 4 · − radical generation and (ii) by promoting the reaction between M(Ca/Fe)–OH and the oxidation products of AsO 4 3− species. These dual effects promoted the formation of Ca 5 (AsO 4 ) 3 OH and FeAsO 4 precipitates that immobilized As(V). Furthermore, the Fe(II)/CaSO 3 system exhibited high resistance against interference from suspended solids and other coexisting substances. The system achieved >98 % removal of 30 mg·L −1 As(III) within 10 min at pH ~12. Notably, the final effluent pH value could be reduced to an ecofriendly value of ~8, and the residual SO 4 2− concentration was lower (140 mg·L −1 ) than that observed in common sulfur-based systems (e.g., peroxomonosulfate, peroxydisulfate, and sodium sulfite). This study presents a perspective shift in treating alkaline wastewater streams by viewing a dominant waste characteristic as a resource rather than as a barrier. Moreover, it provides an effective method for As(III) decontamination of alkaline wastewater.
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高影响因子
Journal of Materials Chemistry A
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2025
·
IF 9.5
Lin-Tao Lv,Zhi-Jie Zhu,Ming-Yuan Shen,Tao Wu,Bin He,Wen-Cui Li
O3-type layered oxides are promising cathode materials for sodium-ion batteries (SIBs). However, their application is limited by tortuous Na+ diffusion channels and complex phase transitions. In this study, a high-rate, low-volume-strain O3-Na0.9Cu0.05Fe0.15Ni0.25Mn0.55O2 (CFNM) cathode is synthesized using a Cu and Fe doping strategy. Multiple characterization techniques and density functional theory (DFT) calculations demonstrate that co-doping modulates the TM-O (transition metal-oxygen) and Na-O bond interactions, expanding Na+ diffusion channels and reducing diffusion energy barriers; the co-doping also promotes electron localization within the TM layers, alters the Na+ deintercalation sequence, and mitigates structural degradation, thereby facilitating rapid and reversible O3-P3 phase transitions without monoclinic phase transitions. The lattice parameter changes exhibit characteristics similar to those of a solid solution, featuring a minimal volume change of 1.1%. Consequently, CFNM delivers a specific capacity of 85.5 mA h g-1 at 10 C and retains 85.2% capacity after 500 cycles at 5 C. Additionally, the full cell assembled with hard carbon (HC) achieves an energy density of 322.8 Wh kg-1 and retains 76.4% capacity after 200 cycles at 1 C. Excellent air stability further demonstrates the practical applicability of CFNM. This study provides new insights into the development of high-performance cathode materials for SIBs.
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高影响因子
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2025
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IF 4.6
Rui Zhou,Miao Dong,Yiwei Wu
N, Si, S co-doped graphene quantum dots (N, Si, S-GQDs) were synthesized from waste toner and glutathione (GSH) via a one-pot hydrothermal method. Combined with o-phenylenediamine (OPD), a rapid, visual, and autocatalytic ratiometric fluorescence sensor of N, Si, S-GQDs/OPD was fabricated for detecting Ag(I) and Fe(III) ions by producing 2,3-diaminophenazine (oxOPD) under pH 8, which emits yellow fluorescence at 560 nm while quenching the blue fluorescence of N, Si, S-GQDs at 440 nm due to an inner filter effect. With the increase of Ag(I)/Fe(III), the blue fluorescence of N, Si, S-GQDs at 440 nm was gradually weakened, along with the enhancement of yellow fluorescence at 560 nm. Hence, this color change from blue to yellow under UV light enables semi-quantitative visual detection. The sensor demonstrates high sensitivity with detection limits of 0.016 µg mL −1 for Ag(I) and 0.010 µg mL −1 for Fe(III), and it successfully detects these ions in lake and tap water without pretreatment. The autocatalytic mechanism involves Ag(I) and Fe(III) reduction to Ag nanoparticles and Fe(II), respectively, which further catalyze the reaction, enhancing selectivity and efficiency. The method is cost-effective, simple, and suitable for on-site environmental monitoring.
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DOI
PubMed
高影响因子
Frontiers in Chemistry
·
2019
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IF 3.782
Xiao Yifan,Deng Sihui,Li Meng,Zhou Qixing,Xu Libang,Zhang Huaifang,Sun Dongmei,Tang Yawen
A feasible and green sol-gel method is proposed to fabricate well-distributed nano-particulate Fe-Ni2P incorporated in N, P-codoped porous carbon nanosheets (Fe-Ni2P@N,P-CNSs) using biomass agarose as a carbon source, and ethylenediamine tetra (methylenephosphonic acid) (EDTMPA) as both the N and P source. The doped Fe in Ni2P is essential for a substantial increase in intrinsic catalytic activity, while the combined N,P-containing porous carbon matrix with a better degree of graphitization endows the prepared Fe-Ni2P@N,P-CNSs catalyst with a high specific surface area and improved electrical conductivity. Benefiting from the specific chemical composition and designed active site structure, the as-synthesized Fe-Ni2P@N,P-CNSs manifests a satisfying catalytic performance toward both oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) in an alkaline solution, with low overpotential, small Tafel slope and long-term durability, relative to the counterparts (Fe-free Ni12P5/Ni2P2O7@N,P-CNSs and CNSs) with single components and even comparable to Pt/C and RuO2 catalysts. The present work broadens the exploration of efficient bifunctional oxygen electrocatalysts using earth abundant biomass as carbon sources based on non-noble metals for low cost renewable energy conversion/storage.
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PubMed
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
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2021
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IF 7.46
Jun Yao,Zhuang Xie,Xiang Zeng,Li Wang,Tingting Yue
Cholesterol is one of the most significant indicators to assess health status. Lanthanide metal-organic frameworks (Ln-MOFs) have a unique luminescence mechanism, which makes it possess tremendous potential in biomonitoring. Thus, on the basic of intramolecular charge transfer theory and quenching effect, the metal-organic frameworks (MOFs) doped by europium was constructed to respond to the cholesterol in serum. The charge transfer direction and the sensing mechanism of fluorescent probe were explained in detail by cross-corroboration of experiment and calculation. The possible sensing mechanism was explained at the molecular level with density functional theory (DFT). With the excitation of 350 nm, the emission peaks at 458 nm and 615 nm which corrsponded to MIL-53(Fe) and Eu centers, appeared enhancement and quenching respectively. To investigate the emission law, the density of states and partial density of states were used to explain the internal electron migration of the probe and the possible sensing mechanism. The results showed the electron transfer efficiency of MIL-53(Fe) was enhanced after Eu 3+ doping, which brought a remarkable improvement in response sensitivity. Meanwhile, the higher energy possessed by the excited state of Eu will lead to the capture of its own electrons by hydrogen peroxide, thus reducing the number of electrons returned to the ground states of Eu and eventually leading to the fluorescence quenching of 615 nm. We anticipate the proposed research is to be an emerging method in cholesterol determination and have further development in all walks of life.
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高影响因子
WASTE MANAGEMENT & RESEARCH
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2024
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IF 3.7
Yan Zhou,Wenhui Liu,Dandan Chen,Bangwei Liu,Ping Lu,Yiwei Zhang
A novel Fe/Ca-modified biochar (BC) derived from corn stalk was prepared in this study for the simultaneous adsorption and immobilization of arsenic, cadmium and lead in aqueous solution and soil, respectively. The adsorption experiment in aqueous solution indicated that 1Ca-Fe@BC exhibited excellent removal efficiency (R, %) towards arsenic (46.3%), cadmium (76.3%) and lead (93.6%). The presence of cadmium and lead could enhance the adsorption efficiency of arsenic by facilitating the formation of ternary complexes with it. Moreover, both cooperative and competitive effects occurred between cadmium and lead adsorption. When the distribution coefficient of cadmium and lead was equimolar, cooperative adsorption prevailed. However, when the distribution coefficient deviated from this balance, competitive adsorption dominated with a higher affinity for lead. The soil culture experiment demonstrated that the utilization of 1Ca-Fe@BC could enhance the stability of arsenic, cadmium and lead in soil by enhancing soil cation exchange capacity and pH while reducing dissolved organic carbon. The competitive and cooperative effects of arsenic, cadmium and lead in soil were consistent with those found in aqueous solution. The results showed that 1Ca-Fe@BC exhibited an excellent remediation efficiency for both arsenic, cadmium and lead-contaminated aqueous solution and soil.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
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IF 9.136
Baicheng Yuan,Xinyi Huang,Shaojinlin Yang,Yi Yang,Zhihong Lin,Raphael Semiat,J. Paul Chen
Heavy metal contamination has become one of the greatest global environmental problems. In this study, a magnetic calcium-alginate hydrogel-sphere encapsulated with Fe–Mn–Zr ternary-metal composite (MCHETC) was prepared through a combined co-precipitation and extrusion approach and used for the adsorption of heavy metals in aqueous solutions. The active sites were dispersed in the MCHETC, which can be separated by the magnetic force for the ease in operation. Above 80% of ultimate adsorption was completed at a contact time of 5 h. The copper uptake history was well described by the intraparticle surface diffusion model, suggesting a multi-step process for the adsorption. The optimum pH for adsorption was 4; the maximum adsorption capacity was 103.1 mg-Cu/g. The adsorption capability well remained after the 5 adsorption–desorption cycles and the copper could be recovered. Furthermore, the adsorbent performed well in the nature water spiked with copper ions. The mechanism studies illustrated that the adsorption was mainly controlled by the ion-exchange reaction. This study demonstrated that the MCHETC adsorption technology may be used for heavy metal removal and recovery with higher efficacy.
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高影响因子
ChemNanoMat
·
2022
·Vol. 8
·期 6
·e202200085
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IF 3.82
Yang Gu,Chuqian Meng,Shuyue Dong,Hexin Zhu,Qian Liu,Yonglan Luo,Qingquan Kong,Tingshuai Li
High-performance earth-abundant electrocatalysts for oxygen evolution reaction (OER) are highly desirable. In this report, we successfully synthesized amorphous Fe−P shell electrodeposited on Co(OH)F nanowire arrays supported on titanium mesh (Fe−P@Co(OH)F/TM) as an efficient catalyst for OER. Such catalyst exhibits excellent OER activity with a low overpotential of 267 mV to reach the geometrical current density of 10 mA cm −2 in 1.0 M KOH. In addition, it has good electrochemical durability to maintain its activity for at least 20 h.
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高影响因子
WATER ENVIRONMENT RESEARCH
·
2020
·Vol. 92
·期 8
·1142-1151
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IF 1.369
Jingyao Huang,Muhammad Danish,Xihao Jiang,Ping Tang,Qian Sui,Zhaofu Qiu,Shuguang Lyu
The performance of trichloroethylene (TCE) degradation by sodium percarbonate (SPC) activated with Fe(II) in the presence of 3.0 g/L sodium dodecyl sulfate (SDS) as well as the role of SDS in the SPC/Fe(II) system was investigated since SDS is a common surfactant used in groundwater remediation for improving TCE dissolution to the aqueous phase. The results showed that though the introduction of SDS could inhibit the TCE degradation, the inhibiting effect was less with the increasing SDS dose. In the presence of SDS, TCE could be completely removed with the SPC/Fe(II)/TCE molar ratio of 40/80/1. Experiments with free radical probe compounds and radical scavengers elucidated that TCE was mainly oxidized by both HO· and . A weakly acidic environment was more favorable to TCE degradation. Nevertheless, at a high concentration had a strongly inhibitive effect on the TCE degradation but the influence of Cl − was negligible. Finally, the excellent TCE degradation achieved in actual groundwater demonstrated that Fe(II) activated SPC technique was applicable in the remediation of TCE contaminated groundwater in the presence of SDS. Practitioner points The effects of SDS were evaluated SPC/Fe(II)/SDS system applied to remediate TCE The mechanism of HO· and generation had been investigated Cl − and affected TCE degradation at different levels The performance of TCE removal in actual groundwater had been studied
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