CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Ting Li,Xiaomeng Wang,Yanmei Chen,Jianru Liang,Lixiang Zhou
Heterogeneous Fenton has become a promising economical and environmentally-friendly method for water treatment, however, the production of abundant radical resources (e.g., O 2 − , OH) are oftentimes limited by finite Fe 2+ species to activate H 2 O 2 . Therefore, development of a new iron-bearing solid modified with diverse functional groups for generating a large of radicals in heterogeneous Fenton is significance. Here, we constructed a Fe 3 O 4 -modified schwertmannite (Fe 3 O 4 /Sch) catalyst to activate H 2 O 2 , SO 4 2− and O 2 to produce three kinds of radicals in heterogeneous Fenton reaction. Specifically, Fe 3 O 4 /Sch catalyst was synthesized to improve its surface properties such as the contents of surface Fe 2+ species as H 2 O 2 or O 2 activators to produce OH or O 2 − , the SO 4 2− of Sch surface as SO 4 − precursor, and electron transfer between Fe 3+ and Fe 2+ . Degradation rate of ciprofloxacin (CIP) for 6 min was up to 97% in Fe 3 O 4 /Sch-H 2 O 2 system, which was higher than that in Sch-H 2 O 2 or Fe 3 O 4 -H 2 O 2 . After four successive cyclic experiments, degradation rate of CIP was still achieved 97% within 10 min in Fe 3 O 4 /Sch-H 2 O 2 system. The formation pathways of the relevant active radicals and the degradation pathways of CIP were also proposed by theoretically calculated and LC-MS data. This finding has not only developed an efficient heterogeneous Fenton catalyst, but also given a new idea of SO 4 − generation by modified iron oxyhydroxysulfate mineral for application of heterogeneous Fenton technology.
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JOURNAL OF SOLID STATE CHEMISTRY
·
2021
·
IF 3.498
Jie Ding,Xiaoxuan Yuan,Jinfeng Wang,Wenfeng Mao,Jianzhong Huo,Jingbo Zhang
Metal-Organic Frameworks (MOFs) have attracted much attention due to its large specific surface, flexible porosity and unsaturated coordination bonds. Cathodic deposition is a unique in-situ potential-driven synthesis method for the deposition of thin film MOFs; however, the gradually consumption of reactants during cathodic deposition might lead to unstable and uncontrollable reaction during thin-film MOF deposition. Herein, oxygen is selected as the initial reactant for the formation of OH − , which can result in gradually and successive formation of thin-film MAF-66 (Metal azolate framework-66), and the particle size and film thickness of the MAF-66 film can be easily tuned by the deposition time. Furthermore, the cathodic deposited thin-film MAF-66 show good adsorption property for heavy metal ions , with Cd 2+ as a representative species. The adsorption capacity can reach 32.3 mg/g (removal ratio: 69%) and the deposited MAF-66 film can achieve a satisfactory recovery degree with structural and morphological stability. In this way, a novel, environmental-friendly, and controllable cathode deposition method is developed for preparation of thin-film MAF-66, which also show great promise as a candidate for heavy metal ions adsorbent.
研究领域:
材料科学
·
环境科学
·
化学工程
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CHEMICAL ENGINEERING SCIENCE
·
2026
·
IF 5.1
Yang Wang,Cuilian Sun,Tianxing Wu,Xiujing Xing,Wei Xiong,Hao Li
The electrocatalytic nitrite reduction reaction (NO 2 RR) converts harmful nitrite in aqueous media into high value-added ammonia (NH 3 ) under mild conditions, representing a promising technology that integrates environmental remediation and green NH 3 synthesis. However, the NO 2 RR undergoes a complex process involving multi-electron/proton transfer steps. Cu-based catalytic systems are universally plagued by the inherent bottleneck of insufficient activity and selectivity, and these dual constraints can hardly be simultaneously overcome by single-element doping alone. Herein, we fabricated fluoride and cobalt co-doped Cu 2 (OH) 2 CO 3 nanosheet catalysts via a one-step hydrothermal method, where the synergistic effect between anionic and cationic dopants enables the simultaneous tailoring of the electronic structure and active site distribution of the material. Electrochemical test results demonstrate that F and Co co-doping can significantly boost the NO 2 RR catalytic performance of Cu 2 (OH) 2 CO 3 . The optimal F-3 sample achieves the highest NH 3 Faradaic efficiency (FE) of 96.47% with an NH 3 yield rate of 28.55 mg h −1 mg cat -1 at −0.8 V (vs. RHE) in 0.15 M NaNO 2 neutral electrolyte, showing a nearly 2-fold performance improvement over the undoped counterpart and outperforming most reported non-noble metal NO 2 RR electrocatalysts. This work provides a high-performance NO 2 RR electrocatalyst for neutral aqueous systems, and demonstrates that anion-cation synergistic doping can break the intrinsic performance bottleneck of Cu-based hydroxyl compounds, offering a valuable modification strategy for rational catalyst design towards electrocatalytic nitrogen-containing pollutant conversion.
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Nature Communications
·
2026
·
IF 18.1
An Yechen,Mei Liang,Yang Ruijie,Cui Jun,Zhang Wenhai,Han Jing-Long,Jiang Wenli,Ren Ruiyun,Gao Xiaoxu,He Zhihui,Xu Haoran,Yan Ruifeng,An Quan-Fu,Li Zhiling,Cheng Haoyi,Tao Yu,Wang Aijie,Zeng Zhiyuan
Membrane-based separation offers a sustainable route for resource recovery from high-salinity organic wastewater, yet graphene oxide (GO) membranes remain constrained by poor selectivity, limited solvent stability, and challenges in scale-up. Here, we report a hydroxylated single-walled carbon nanotube (SWCNT-OH) reinforced GO membrane, in which SWCNT-OH promotes robust inorganic crosslinking with sodium tetraborate (Na 2 B 4 O 7 ) to form rapid transport channels for water and ions, while suppressing organic passage. This architecture enhances the moxifloxacin (MXF)/NaCl separation factor more than fivefold (from 4.2 to 22.2) and increases water permeability over fourfold (from 7.2 to 30.1 l m −2 h −1 bar −1 ). The membrane was scaled up to 11 m 2 and deployed for continuous treatment of MXF crystallization mother liquor over seven days, delivering a stable recovery of 10 kg MXF per day under industrially relevant conditions. These findings establish a scalable strategy for the design of robust nanocarbon-based membranes, advancing resource-efficient treatment of high-salinity wastewater.
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PubMed
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2026
·
IF 6.7
Xiangyang Gao,Xin Liu,Chenxi Zhou,Qiyan Wang,Ruya Guo
Tailoring efficient bifunctional electrocatalyst with dual-heterojunction is crucial for overall water splitting (OWS). Herein, a multicomponent bifunctional catalyst with dual-heterojunction is rapidly constructed via sequential electrodeposition for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Density functional theory (DFT) calculations reveal that bidirectional electron transfer at the interface induces a double built-in electric field (BIEF) in Pt/CeO 2 -Ni(OH) 2 , which offers additional impetus for electron transport and brings the d -band center closer to the Fermi level, thereby optimizing reaction kinetics and the adsorption of reaction intermediates. Active Pt and CeO 2 nanoparticles (NPs) are uniformly anchored on the stable Ni(OH) 2 nanoflocs, ensuring high exposure of active sites and preventing NPs aggregation. Meanwhile, Ni(OH) 2 , serving as abundant electron donor center, forms dual heterointerface with Pt and CeO 2 (Pt-Ni(OH) 2 and CeO 2 -Ni(OH) 2 ), which ensures structural stability during electrochemical processes. Benefiting from the dual-heterojunction and the unique structure design, Pt/CeO 2 -Ni(OH) 2 exhibits excellent electrocatalytic performance, requiring only 66 mV (10 mA cm −2 ) and 278 mV (100 mA cm −2 ) for HER and OER, respectively. Remarkably, the two-electrode electrolyzer based on Pt/CeO 2 -Ni(OH) 2 electrode requires only 1.49 V to deliver 10 mA cm −2 with an excellent durability for OWS. This work brings light to the rational design and directional construction of bifunctional electrocatalyst hybrid nanomaterials with multiple heterojunctions.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2026
·Vol. 60
·期 32
·22965-22976
·
IF 12.2
Cheng Dong,Ma Runhao,Tan Yuansen,Wu Zhongkuan,Ding Haoran,Wu Fan,Chen Si,Wang Huaqing,Lou Guangyu,Ma Yingying,Wang Binbin,He Feng
Oxygenation
of mackinawite (FeS) at redox interfaces
constitutes
a key biogeochemical process that generates hydroxyl radicals ( • OH) and facilitates contaminant attenuation. However,
the influence of common inorganic ligands such as tripolyphosphate
(TPP) on interfacial electron transfer in this process remains poorly
understood. Herein, 1.0 mM TPP increased cumulative • OH production approximately 23.5-fold over 180 min of FeS oxygenation,
with the electron utilization efficiency for • OH
production increasing from 0.33% to 8.18%. TPP enhanced • OH generation by promoting Fe(II) dissolution, thereby driving homogeneous
Fenton-like reactions, while facilitating Fe(III)/Fe(II) redox cycling
through solid–liquid interactions. Additionally, TPP acted
as an interfacial coordination modulator by rearranging the local
Fe(II) environment, and the resulting surface Fe(II)-TPP complexes
improved the utilization of structural electrons. Electrochemical
measurements and DFT calculations indicated that this interfacial
coordination suppressed structural Fe(II) oxidation and reduced unproductive
electron consumption, while lowering the energy barrier for H 2 O 2 -forming O 2 activation at TPP-modified
FeS sites. XRD, FTIR, and EXAFS analyses showed that TPP adsorption
inhibited lepidocrocite crystallization and redirected secondary mineral
evolution toward ferrihydrite-rich products. These findings elucidate
how ubiquitous ligands regulate mineral-water interfacial processes
and • OH generation, providing a basis for optimizing
FeS-based environmental remediation technologies.
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PubMed
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NANO
·
2024
·
IF 1
Junxiang Mo,Jun Li,Jing Li,Yashan Li
The development of composite materials is a key area of research for enhancing the electrochemical performance of electrode materials. In this study, NiCo–S nanostructured hybrid electrode materials were prepared on nickel foam (NF) by using binary metal–organic frameworks (MOFs) as the sacrificial template through a two-step hydrothermal method. Ni–MOF was then deposited on the surface of NiCo–S/NF through the hydrothermal method and subsequently converted into Ni(OH) 2 through a subsequent alkalization treatment. The duration of the Ni–MOF hydrothermal process was varied as a parameter. NiCo–S@Ni–MOF/NF was prepared through hydrothermal reaction for 6 h, 9 h and 12 h, followed by heating in a 6 M KOH solution at 75 ∘ C for 6 h in a water bath. The electrode materials with the best morphology and electrochemical properties were obtained when the hydrothermal reaction time was 6 h. The optimized electrode had a specific capacity of 2533.2 F ⋅ g − 1 at 1 A ⋅ g − 1 and a capacity retention rate of 60.8% at 10 A ⋅ g − 1 , which indicated good rate performance. Additionally, the electrode material demonstrated excellent cycling stability, with a capacity retention rate of 95.3% after 5000 cycles at 50 mV ⋅ s − 1 . The energy density of the hybrid supercapacitor device assembled from this electrode material was 33.5 Wh ⋅ kg − 1 when the power density was 849.89 W ⋅ kg − 1 at a current density of 1 A ⋅ g − 1 .
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ACS Sustainable Chemistry & Engineering
·
2026
·
IF 7.3
Ying Liang,Xianping Liao,Yingshuai Jia,Shiming Guan,Wanling Zhang,Wenbiao Zhang,Yuying Meng,Yi Tang,Qingsheng Gao
Electrooxidation offers a sustainable alternative by utilizing renewable energy to convert biomass-derived cyclohexanol (CHA) to adipic acid (AA), a key industrial chemical for nylon-66 and polyurethane production. While bimetallic Ni-based catalysts enhance the conversion, the role of secondary metals in modulating Ni active-site reconstruction during operation remains unclear, limiting performance optimization. Here, we demonstrate that Cr-doping promoted the dynamic reconstruction of Ni(OH)2 nanosheets to form NiOOH with abundant Ni3+ and oxygen vacancies (OVs), significantly boosting AA electrosynthesis. In situ characterizations reveal that Cr-doping accelerates OH– adsorption and promotes NiOOH formation, while subsequent Cr3+ leaching generates OVs, thus, resolving the long-standing dilemma between stabilizing high-valence Ni and maintaining abundant defects. The optimized catalyst achieves 78.1% AA yield and 85.4% Faradaic efficiency at 1.45 V vs RHE, outperforming undoped Ni(OH)2 and prior systems. Mechanistic studies identify surface Ni3+ and OVs-stabilized *OOH species as the keys for CHA dehydrogenation and cyclohexanone oxidation, respectively. Moreover, a membrane electrode assembly electrolyzer was designed for the efficient coproduction of AA (0.078 mmol h–1 cm–2) and H2 (42.9 mL h–1 cm–2) at a current density of 100 mA cm–2, demonstrating the scalability. This work clarifies the in situ reconstruction of bimetallic sites and provides a design strategy for the efficient electrosynthesis.
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JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES
·
2026
·Vol. 131
·期 18
·e2026JD047458
·
IF 3.8
Ruidong Zhang,Kun Li,Yifan Zhou,Li Xu,Aijing Song,Jie Hu,Xiaowen Chen,Kuanyun Hu,Xueqi Ma,Huiwen Ding,Jianlong Li,Lin Du
Biomass burning (BB) emits large amounts of polycyclic aromatic hydrocarbons (PAHs) and is an important source of secondary organic aerosol (SOA). Recent studies suggest that, compared with gas-phase oxidation, the oxidation of BB-emitted organics in atmospheric aqueous phases can substantially enhance the formation of aqueous SOA (aqSOA). However, the aqueous-phase transformation and environmental fate of PAHs from BB remain poorly understood. This study reports the OH-initiated aqueous-phase oxidation kinetics and reaction mechanisms of three representative biomass-burning PAHs: naphthalene (NAP), acenaphthene (ACE), and acenaphthylene (ACY). The second-order aqueous-phase rate constants for reactions with OH were measured to be (1.63 ± 0.55) × 10 10 , (3.37 ± 1.15) × 10 10 , and (2.07 ± 0.70) × 10 10 M −1 s −1 for NAP, ACE, and ACY, respectively. The estimated aqueous-phase lifetimes were generally shorter than the corresponding gas-phase lifetimes under the representative OH conditions considered here, highlighting the potential importance of atmospheric aqueous environments in promoting the aging and transformation of these PAHs. Product analysis and pathway inference showed that NAP and ACE preferentially formed lower-carbon, more highly oxidized products, whereas ACY more readily produced oxygenated products that retained larger carbon skeletons. Furthermore, this study identified six previously unreported aqueous-phase oxidation products, reflecting ongoing oxidation and structure-dependent patterns of product evolution. Field observations showed that five newly identified products were also detected in ambient PM 2.5 samples, supporting the atmospheric relevance of the laboratory-identified products. These results improve our understanding of the aqueous-phase transformation of PAHs and their potential contribution to aqSOA formation.
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Materials Today Chemistry
·
2026
·
IF 7.4
Dahong Peng,Hongkang Su,Ziting Yan,Chenxu Li,Shilie Pan,Min Zhang
A systematic comparison of F − /OH − modified [B 3 O 6 ] 3- clusters shows that properties evolve with F − /OH − content. • By changing the type and arrangement of the fundamental building blocks, a breakthrough in dimensionality was achieved. • Tunable optical properties were achieved, namely, the birefringence across the series ranges from 0.013 to 0.112 at 546 nm. Borates stand out as a prominent class of compounds in structural chemistry, acclaimed for their extraordinary structural diversity stemming from the versatile B–O fundamental building blocks (FBBs), and terminal oxygen modification has emerged as a powerful and effective strategy for tailoring their structures and optimizing functional properties. Herein, we report the synthesis of seven novel hydroxyfluorooxoborates with different dimensional framework via F − /OH − terminal modification of the isolated [B 3 O 6 ] 3- cluster, aiming to explore structural diversity and structure-property relationships. These compounds are classified by their FBBs: Compounds I-IV (A 7 [B 3 O 3 F 4 OH] 2 (PF 6 ) 3 , A = Rb, K, Cs, NH 4 ) with [B 3 O 3 F 4 (OH)] 2- ; Compounds V-VI (Cs 1.2 (NH 4 ) 0.8 [B 3 O 3 F 2 (OH) 2 ] 2 and Rb 1.7 K 0.3 [B 3 O 3 F 2 (OH) 2 ] 2 ) with [B 3 O 3 F 2 (OH) 2 ] - ; and Compound VII (Rb 7 [B 3 O 3 F 2 (OH) 2 ] 2 [B 3 O 3 F 4 (OH)](NO 3 ) 2 BF 4 ) with coexisting [B 3 O 3 F 4 (OH)] 2- and [B 3 O 3 F 2 (OH) 2 ] - . The birefringence across the series ranges from small (∼0.013 - 0.024 at 546 nm for I-IV) and moderate (∼0.051 at 546 nm for VII) to large (∼0.063 - 0.112 at 546 nm for V and VI). Structural and properties analyses reveal that F − /OH − substitution eliminates B–O dangling bonds of [B 3 O 6 ] 3- , leading to varied [B 3 O 3 F 2x (OH) 3−x ] (x = 1, 2, 3) and [B 3 O 3 (OH) x ] (x = 3, 4, 5, 6), featuring a distinct structure-property relationship. In the [B 3 O 3 (OH) x ] series, both polarizability anisotropy and band gap decrease with rising hydroxyl content, while hyperpolarizability increases. In contrast, the mixed F − /OH − series exhibit the opposite trend. In conclusion, this work significantly provides a rational synthetic strategy for tailoring FBBs and constructs deep-ultraviolet hydroxyfluorooxoborates with tunable optical performance. Through F − /OH − terminal modification of [B 3 O 6 ] clusters, a structural breakthrough from 0D clusters to a 2D layer was achieved, along with tunable optical properties. Download: Download high-res image (251KB) Download: Download full-size image
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Waste and Biomass Valorization
·
2026
·
IF 3.1
Zhao Kunzhen,Zhang Zhuoma,Hang Xina,Yi LinLin,Li Kaiyuan,Zou Yanyan
Polyether ether ketone (PEEK) is a high-performance thermoplastic with considerable potential for H 2 and syngas productions via pyrolysis. However, its conventional non-catalytic pyrolysis suffers from high energy consumption and low H 2 and syngas yields. This study investigates the catalytic pyrolysis of PEEK using nickel hydroxide (Ni(OH) 2 ) to enhance the gas production efficiency. PEEK mixed with Ni(OH) 2 at different molar ratios (1:0–1:2) was pyrolyzed up to 1073 K under a nitrogen atmosphere. The H 2 yield increased with catalyst loading and reached a maximum of 25.9 mg/g at a PEEK: Ni(OH) 2 ratio of 1:0.5 (13.85 wt%), corresponding to a 264.3% increase compared with non-catalytic pyrolysis. The syngas yield also reached a maximum of 0.75 g/g under the same condition. Thermogravimetric analysis showed that the addition of Ni(OH) 2 significantly lowered the onset decomposition temperature of PEEK from 832 K to 532 K, and transformed its two-stage pyrolysis into a four-stage process with a 10.4% reduction in char residue. In-situ X-ray diffraction revealed that Ni(OH) 2 was progressively transformed into NiO and Ni during heating, indicating the formation of catalytically relevant Ni-containing phases within the pyrolysis temperature range. Scanning electron microscopy showed that the catalyst was distributed within the carbon matrix and altered the morphology of the pyrolysis residue. These observations provide qualitative evidence of morphological changes after catalytic pyrolysis. These findings demonstrate that the catalytic potential of Ni(OH) 2 in facilitating H 2 -rich syngas production from PEEK.
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APPLIED SURFACE SCIENCE
·
2026
·
IF 6.6
Rongjing Jia,Shuling Chang,Ruirui Wang,Yanhong Xu,Rijie Wang,Lihong Zhang
The electrocatalytic CO 2 reduction reaction to CO (ECO 2 RR) is an effective way to achieve carbon resource utilization. It requires catalysts that can synergistically couple CO 2 activation with efficient CO desorption. This work engineers this synergy by constructing an interfacial Ag δ+ -O-Zn configuration on Zn(OH)F-derived supports via controlled Ag loading (0–5 wt%). The optimal catalyst (3A/Z, 3 wt% Ag) balances the formation of interfacial, oxidized Ag species (Ag δ+ ) with well-dispersed metallic Ag 0 nanoparticles. It achieves a CO Faradaic efficiency of 95.4% at −1.15 V vs. RHE and maintains 86% efficiency over 5 h at 6.38 mA cm −2 . In-situ ATR-SEIRAS spectra and kinetics reveal that Ag δ+ -related sites lower the barrier for *COOH formation, while adjacent Ag 0 domains facilitate *CO desorption. Excessive loading (5A/Z) promotes Ag aggregation and support decomposition, diminishing the critical Ag δ+ -O-Zn interface and performance. This study highlights interface coordination engineering as a key strategy for designing bifunctional ECO 2 RR catalysts.
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