CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Junjie Chen,Xiaomei Xing,Sisi Wen,Mengyuan Li,Di Liu,Wenji Jiang,Xinyi Shao,Ruikai Qi,Yumei Yang,Ming Mu,Zheng-jie Chen,Bing Zhao,Wei Song
The pursuit of efficient ammonia production through electrochemical nitrate reduction reaction (NO 3 RR) at ambient conditions is a significant demand in green and energy-saving industries. Rational tailoring of the competing yet complementary processes of water splitting and nitrate activation at reducing potentials is pivotal for manipulating the efficiency and selectivity of ammonia synthesis. Herein, Ag 92 Ru 8 aerogel has been synthesized via a one-step reduction strategy, demonstrating remarkable in tuning the reaction intermediates and interfacial water dynamics. Based on Ag 92 Ru 8 aerogels, a high NH 3 Faradaic efficiency (FE) of 97.16 %, and a superior yield rate of 2.49 mmol h −1 mg cat. −1 were achieved at −0.5 V . And the corresponding Zn-NO 3 − battery exhibited potential as a power source for practical application. In-situ surface-enhanced Raman spectroscopy (SERS) and density functional theory (DFT) results demonstrate that H* intermediate generated from interfacial water are promoted by Ru species in the hydrogenation process of NO 3 RR, offering valuable insights for the targeted design of efficient catalysts.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Qin-Hua Xu,Yuxin Li,Junyue Bao,Zeting Li,Yaofeng Cai,Yanbin Xu
The widespread adoption of anaerobic digestion in manure management necessitates handling discharged ammonia–nitrogen (NH 4 + -N)-rich digestate, where electrochemical ammonia recovery is a viable solution but is limited by the cost of membrane fouling. Here, we present a membrane-free ion enrichment electrolyzer (MIEE) engineered with an electrode spatially decoupled structure, enabling NH 4 + and OH – ion enrichment in the anaerobic digestate for further ammonia recovery. Through in-situ measurements, we identify electrochemically induced relative concentration gradients of ions as the pivotal mechanism driving ion enrichment. MIEE maintains electroneutrality by migrating ions, and the effect is close to electrodialysis below ∼50 % migration of NH 4 + ions. Cathode effluent treated by MIEE achieves ∼80 % ratio of NH 4 + -N recovery in the stripping process, coupled with carbon mitigation. The cost of OH – ions supplied by MIEE is ∼50 % compared to directly dosing NaOH. The anode effluent neutralizes the stripping effluent pH from 9.3 to 8.6 and optimizes the organic carbon/nitrogen molar ratio from 1.5 to more than 3, enhancing compatibility with the bioprocess. This study presents a novel strategy for enriching ions without ion exchange membranes, which reduces the cost of membranes and stripping pretreatment in the ammonia recovery.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
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IF 21.1
Zhimo Fang,Yuan Liang,Zepeng Zeng,Haotian Bai,Zhou Zhou,Lin Zhang,Bin Hu,Shiguan Yang,Jihong Li,Qiang Lu
Herein, we synthesized well-dispersed N and Fe-doped CoS 2 (FNCS) with stable sulfur vacancies (S V ) for Fenton-like reaction. The characterization, experimental, and calculation results jointly unveiled the synergistic modification of heteroatoms and defects within FNCS constructed unique Co−N−Fe···S V sites, enabling synchronous activation of peroxymonosulfate (PMS) and dissolved oxygen (DO). Optimized S 3p-Co 3d orbital hybridization facilitated efficient electron cycling, generating both SO 4 •− radicals and singlet oxygen ( 1 O 2 ) at Co−N−Fe···S V sites. Consequently, the FNCS/PMS system, operating via a radical-nonradical synergistic mechanism, achieved an ultra-high pollutant degradation rate constant of 2.71 min⁻¹ , 3.77 times higher than radical-dominated CoS 2 /PMS, while retaining over 90 % of its initial activity after 10 h of operation with strong interference resistance. This work provides a clear perspective on regulating the electronic structure of active sites to synergistically activate multiple oxidants for enhanced Fenton-like catalysis.
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Nature Communications
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2025
·Vol. 16
·期 1
·1-12
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IF 15.7
Zhou Yuanbo,Zhang Lifang,Wang Mengfan,Shen Xiaowei,Zhu Zebin,Qian Tao,Yan Chenglin,Lu Jianmei
High-entropy alloys, with their unique structural characteristics and intrinsic properties, have evolved to be one of the most popular catalysts for energy-related applications. However, the geometry of the traditional nanoparticle morphology confines the majority of active atoms to the particle core, deeming them ineffective. In this study, we present a class of two-dimensional high-entropy alloys, namely, high-entropy metallenes, constructed by alloying various single-atom metals in atomically thin layers and reveal their great feasibility for electrocatalytic nitrate reduction to ammonia. Through multimetal interactions, various active centres are formed and sufficiently exposed over the metallene. Each element performs its own duties and jointly lowers the energy barrier of the rate-determining step. As expected, the proof-of-concept PdCuNiCoZn high-entropy metallene delivers satisfactory catalytic performance across wide pH ranges. In particular, in a strongly alkaline electrolyte, a maximum ammonia yield rate of 447 mg h −1 mg −1 and a high Faradaic efficiency of 99.0% are achieved.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2025
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IF 11.3
Yu Lei,Chen Cheng,Yangjian Zhou,Xiaoran Chen,Xin Lei,Wenjing Song,Zhimin Qiang,Chuncheng Chen,Jincai Zhao
More frequent global wildfire events intensify the exposure risks of nitrophenols through brown carbon (BrC) emissions. Radical reactions dominate the fates of nitrophenols in surface, municipal, and atmospheric waters, yet the involved reaction kinetics and mechanisms remain poorly understood. In this work, by combining transient and steady-state multispectral analyses, the second-order rate constants (k) for nitrophenols and biomass-burning BrC reacting with HO• as well as common secondary radicals (e.g., Cl2•–, CO3•–, and NO3•) were determined (k ≈ 105–1010 M–1 s–1 at pH 2.0–10.0 for both protonated and deprotonated nitrophenols), most of which are reported for the first time. We also experimentally demonstrated that the reactions of nitrophenols and BrC with various radicals could produce a substantial amount of HONO/NO2– (a key precursor of tropospheric HO•), with molar yields reaching ∼50%. Mechanistic investigations revealed that the phenoxy radical (PhO•), generated from either single electron transfer or addition–elimination reactions during the radical reactions of nitrophenols, acted as a universal intermediate for the denitration. Hence, the new kinetic and mechanistic insights suggest that the radical-induced denitration process of BrC and nitrophenols in acidic waters may serve as a previously overlooked HONO source, but such denitration does not guarantee detoxification due to the simultaneous generation of high-risk biphenols. This work highlights the critical role of secondary radicals in nitrophenols and BrC transformation across different waters, shedding light on several unforeseen chemical impacts driven by intensified global wildfires.
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ADVANCED FUNCTIONAL MATERIALS
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2025
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IF 19
Lixue Zhou,Daming Feng,Zhiqiang Li,Hui Li,Chunhua Ge,Xiangdong Zhang,Tianyi Ma
High-entropy materials offer unique advantages in catalysis due to lattice distortion, compositional complexity, and entropy-driven stability. In this study, we report a crystal phase-engineered high-entropy perovskite oxide, LaB 5 O 3 (B═Fe, Cu, Co, Cr, and Ni), which enables efficient bifunctional electrocatalysis. Structural transformation from orthorhombic to cubic symmetry modulates the spin states of B-site metals, particularly stabilizing the high-spin state of Fe 2 ⁺/Fe 3 ⁺, enhancing electron density and nitrate adsorption. This leads to a NH 3 Faradaic efficiency (FE) of 95.83% at −0.7 V vs. RHE for nitrate reduction (NO 3 RR), with minimal NO 2 ;− byproduct (FE < 2%). Concurrently, LaB 5 O 3 exhibits excellent sulfide oxidation reaction (SOR) activity, requiring only 0.484 V vs. RHE at 10 mA cm −2 —considerably lower than oxygen evolution reaction (OER) overpotential. Integrated into a paired electrolyzer, the system achieves simultaneous nitrate-to-ammonia conversion (max FE: 81.27%) and sulfide-to-sulfur transformation at a cell voltage of just 1.079 V. The superior performance arises from synergistic effects of high-entropy design, including enhanced oxygen vacancy formation, lattice strain, and ferroelectricity. This work demonstrates the potential of crystal phase engineering in high-entropy oxides for sustainable nitrogen fixation and sulfur recovery in water treatment applications.
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WATER RESEARCH
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2025
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IF 12.4
Zhengwei Pan,Guohao Geng,Sanchuan Yu,Hongwei Lu,Meihong Liu,Doufeng Wu,Congjie Gao
Polyamide (PA) reverse osmosis (RO) membranes face persistent challenges including the trade-off between permeance and selectivity, limited chlorine resistance, and insufficient long-term stability. In this work, these challenges were addressed by developing a synergistic modification strategy in which Fenton oxidation facilitates the grafting of aromatic amine monomers, with p-aminobenzenesulfonamide (SAs), p-aminobenzoic acid (PABA), and p-aminobenzenesulfonic acid (SFA) as functional modifiers, marking the first application of this approach in membrane modification. This approach introduces phenazine-based quinone imine structures and additional functional groups onto the membrane surface, facilitating rearrangement of aromatic ring stacking from “π-π” to “T-π” configurations within the PA molecular backbone, while simultaneously modulating surface hydrophilicity and charge. As a result, water permeance increases from 4.91 to 6.01 L·m -2 ·h -1 ·bar -1 , NaCl permeance decreases from 0.373 to 0.201 L·m -2 ·h -1 , and perm-selectivity (A/B) rises from 14.8 to 24.4 bar -1 for PA-PABA membranes. Notably, modified membranes maintain NaCl rejection above 98.50% even after 50,000 ppm·h of active chlorine, with PA-SAs showing particularly robust chlorine resistance, far superior to conventional PA membranes. These results highlight that Fenton-assisted aromatic amine grafting, based on aqueous-phase reactions, low energy consumption, and scalable grafting monomers, provides a new approach for the scalable fabrication of high-performance RO membranes, holding significant industrial potential and offering a promising solution to extend membrane operational lifetimes in advanced water treatment applications.
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Applied Sciences-Basel
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2025
·Vol. 15
·期 24
·12861
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IF 2.5
Jianzhang Wang,Yingxia Wu,Jian Zhang,Shengli Wang,Hongliang Wang
Featured ApplicationIn this study, a traveling nutrient analyzer was designed for real-time, in situ monitoring of nutrients in seawater from moving vessels or fixed observation stations. It is a reliable tool for oceanographic surveys, marine environmental protection, and ecological research, enabling high-frequency data acquisition that is essential for understanding dynamic marine biogeochemical processes.Continuous monitoring of seawater nutrients is crucial for marine resource research and conservation, yet it faces challenges due to the constraints of offshore working conditions. We developed a multi-analyte sensor based on flow analysis technology, which integrates wet-chemical colorimetry/fluorometry for the simultaneous in situ determination of nitrite, nitrate, ammonium, silicate, and phosphate in seawater. To mitigate bubble interference, an integrated gas-trapping cavity was designed, and a data-cleaning algorithm based on the interquartile range method was implemented. In June 2025, a sea trial was conducted at two stations in the northern South China Sea, the results of which showed high consistency with laboratory standard methods: the maximum absolute relative errors were 1.79% for nitrite, 5.01% for nitrate, 1.42% for ammonium, 5.93% for phosphate, and 2.95% for silicate. The performance under real marine conditions is demonstrated by relative errors below 6% and linear correlation coefficients exceeding 0.999 for all parameters. This research demonstrates a practical approach for in situ marine observation.
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Nature Protocols
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2025
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IF 16
Dong Kai,Han Shuhe,Li Yanan,Wang Zhongliao,Xue Chuang,Sun Xiaogang,Yao Yongchao,Li Haobo,Wang Xin,Ma Dongwei,Liu Li-Min,Zhang Bin
The electrocatalytic nitrate reduction reaction (NO 3 RR) has emerged as a promising approach for sustainable nitrogen management, enabling the selective conversion of nitrate into targeted nitrogen-containing compounds, such as ammonia and hydroxylamine. However, the efficiency and selectivity of the NO 3 RR are highly dependent on the physicochemical properties of the electrocatalysts, necessitating a standardized and comprehensive characterization protocol. Here we provide a detailed methodology for the structural, chemical, electronic and electrochemical characterization of the materials used in the NO 3 RR. We outline procedures for evaluating catalyst morphology, composition and redox states, as well as methodologies for quantifying reaction products to determine nitrate conversion efficiency and selectivity. To track catalyst evolution and reaction pathways under reaction conditions, we present real-time monitoring strategies that capture structural changes, key reaction intermediates and electronic transformations associated with chemical bond formation and cleavage. In addition, we incorporate theoretical calculations to comprehensively evaluate the reaction pathways and their interplay with the electronic structures of electrocatalysts, providing deeper mechanistic insights into the reaction kinetics, active site evolution and selectivity-determining factors. This Protocol is designed for researchers in electrocatalysis, environmental chemistry and energy conversion, offering a reproducible workflow for catalyst assessment. The step-by-step methodology ensures reliable data collection and interpretation, enabling direct comparisons across different catalysts and facilitating the development of more efficient NO 3 RR catalysts. The entire workflow requires ~8–10 days, depending on sample preparation and measurement duration.
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Surfaces and Interfaces
·
2024
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IF 5.7
Zhiwei Zou,Hongxiang Zhang,Xuefeng Pan,Hui Shen,Jianying Yu,Tengfei Guo,Yonghao Wang
Electrocatalytic reduction of nitrate (NO 3 - ) to ammonium (NH 4 + ) is an environment friendly approach for treating nitrogen-containing wastewater. Consequently, electrocatalysts capable of effectively and selectively reducing NO 3 - to NH 4 + receives growing attention. However, Cu-based catalysts demonstrate limited efficiency and the drawback of generating toxic NO 2 - though it is prevalent in the field of electrocatalytic reduction of NO 3 - (NO 3 RR). In this work, a CuNi alloy was synthesized on a Co foil through electrodeposition (marked as CuNi@Co) and its electrocatalytic performance for NO 3 RR was evaluated. XRD, EDS mapping and XPS characterization indicate CuNi exists with alloy state. Electrocatalytic experiments demonstrate that CuNi@Co exhibits an exceptional FE NH3 of 99.12% at -0.64 V (vs. RHE). Importantly, no detrimental NO 2 - generated during NO 3 RR process because the reduction rate from NO 2 - to NH 4 + is faster than that from NO 3 - to NO 2 - . Mechanistic analysis suggests that Cu serves as a ‘reservoir’ to provide electrons to facilitate the reduction of NO 3 - to NO 2 - during NO 3 RR process and the synergistic effect of Ni and Cu promotes more active hydrogen (H*) to participate the reduction process of NO 2 - to NH 4 + not H 2 generation, ultimately improving FE NH3 . This work elucidates the role of electrons and H* in electrocatalytic nitrate reduction to ammonium for CuNi alloy, providing new insights into the reduction process of NO 3 RR for Cu-based materials.
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ChemistrySelect
·
2024
·Vol. 9
·期 10
·e202303652
·
IF 1.9
Huanhuan Ma,Na Zhang,Xinzhu Wang,Kui Lin,Ping Liu,Fei Tian
Graphical A green one-step hydrothermal method has been successfully used to prepare carbon dots (CDs) by selectively co-doping nitrogen, phosphorus and sulphur elements. For the sensitive detection of iron ions, a fluorescence quencher sensor based on nitrogen- and sulphur-doped carbon dots (red NS-CDs) has been developed, because of the good optical properties and bio-histocompatibility of green NPS-CDs and blue NP-CDs, They are observed to penetrate NCl−H292 cells, fluorescing green and localizing in the cytoplasm. Carbon dots (CDs) with tunable photoluminescence was successfully prepared via selective co-doping of three elements, including nitrogen, phosphorus and sulfur element by green one-step hydrothermal method. Nitrogen-sulfur-doped CDs (red NS-CDs), which emitted red fluorescence under UV excitation, were used to detect iron ions in the linear range 1–50 μM, yielding detectable limits as low as 94 nM. The nitrogen-phosphorus-doped CDs (blue NP-CDs) exhibited blue fluorescence with quantum yields up to 34.5 %. When the concentration is 800 μg/mL, it showed excellent anticancer effect in vitro. The nitrogen-sulfur-phosphorus-doped CDs (green NPS-CDs) emitting green fluorescence showed a low cytotoxicity at a high concentration of 800 μg/mL and were used for intracelluar imaging of NCl−H292 cells. This study demonstrated the photoluminescent characteristics of carbon dots (CDs) and highlighted the ability to modify their peak fluorescence emission wavelengths through the flexible combination of specific reagents under comparable hydrothermal conditions. Additionally, it provided valuable insights into the efficient methodologies for synthesizing CDs suitable for various application scenarios.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2025
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IF 6
Fengjiao Quan,Pengfei Xu,Xiufan Liu,Wenjuan Shen,Yuhao Li,Jianfen Li,Yun He,Fangyuan Chen
Nitrate (NO 3 − ) pollution in groundwater has emerged as a pressing environmental issue of global concern. The excessive application of chemical fertilizers is widely recognized as the primary contributor to this pollution Nitrate ions pose significant risks to human health and the ecological environment. Electrochemical reduction of NO 3 − to NH 3 (NITRR) represents an effective approach for nitrogen recovery and recycling. Among many electrode materials, copper-based catalysts were considered promising due to their low cost and strong NO 3 − conversion capability. However, excessively strong adsorption can lead to catalyst deactivation, thereby diminishing catalytic activity. In this study, we developed an electrode material (Cu@NiO/NF) with low-valent copper (Cu δ+ ) through the combination of Cu and NiO, and it exhibited excellent catalytic performance in the NITRR process. At − 0.45 V vs. RHE, this catalyst achieved a Faraday efficiency of 95.7 % and an ammonia yield of 0.85 mg h −1 cm −2 . Further experiments and theoretical calculations demonstrate that the presence of NiO in Cu@NiO/NF stabilizes Cu δ+ , thereby enhancing the charge transfer rate and promoting the formation of hydrogen radicals (H•). This work has pioneered a new avenue for the development of efficient and innovative NTIRR materials.
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