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Spin-state engineering via ionic mismatch in MnO2 for high-performance hybrid capacitive deionization 基于离子失配的MnO2自旋态工程用于高性能杂化电容去离子
IF 9.8 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-06-01 Epub Date: 2026-02-25 DOI: 10.1016/j.desal.2026.120024
Xiaoke Li , Jinghua Yang , Xuejing Wang , Shiyu Wang , Jingyu Wu , Ruilong Liu , Guixi Wang , Jun Wang , Weikun Ren , Feike Zhang , Weijie Fu , Yingjie Ji , Zhiyu Yang , Yi-Ming Yan
Manganese dioxide (MnO2) is a promising electrode material for hybrid capacitive deionization (HCDI) due to its high theoretical capacity and low cost, yet the Jahn-Teller (J-T) distortion induced by high-spin Mn3+ ions (t2g3eg1) causes severe structural degradation and manganese dissolution, critically hindering its practical stability. Herein, we report a spin-state engineering strategy via cobalt-induced ionic radius mismatch to intrinsically suppress J-T distortion in MnO2. Co doping induces significant local lattice distortion, thereby breaking octahedral symmetry and inducing crystal field splitting. Systematic density functional theory (DFT) calculations reveal that this lattice distortion-driven crystal field distortion causes a significant upward shift in the Mn dz2 orbital energy level, compelling electron redistribution from eg orbitals to lower-energy t2g orbitals. This electronic reconfiguration effectively transitions Mn3+ from a high-spin to a low-spin state, thereby eliminating the uneven electron occupation in eg orbitals that drives J-T distortion. Consequently, the optimized Co-MnO2 electrode demonstrates superior HCDI performance in 500 mg L−1 NaCl solution: a high initial salt adsorption capacity (SAC) of 83 mg g−1, a rapid salt adsorption rate (SAR) of 4.33 mg g−1 min−1, and remarkable cycling stability with 82% capacity retention after 150 cycles. Experimental characterizations confirm enhanced MnO bond strength and suppressed manganese dissolution, validating the effectiveness of spin-state control. This work establishes ionic radius mismatch as a versatile design principle for developing J-T distortion-resistant electrochemical materials, offering new insights for engineering ultra-durable electrodes in water desalination and beyond.
二氧化锰(MnO2)具有较高的理论容量和较低的成本,是一种很有前途的用于杂化电容去离子(HCDI)的电极材料,但高自旋Mn3+离子(t2g3eg1)引起的Jahn-Teller (J-T)畸变导致严重的结构降解和锰溶解,严重阻碍了其实际稳定性。在此,我们报告了一种通过钴诱导离子半径失配的自旋态工程策略,从本质上抑制MnO2中的J-T畸变。Co掺杂引起明显的局部晶格畸变,从而破坏八面体对称性,引起晶体场分裂。系统密度泛函理论(DFT)计算表明,这种晶格畸变驱动的晶体场畸变导致Mn dz2轨道能级显著上升,迫使电子从eg轨道重新分布到能量较低的t2g轨道。这种电子重配置有效地将Mn3+从高自旋态转变为低自旋态,从而消除了导致J-T畸变的eg轨道上不均匀的电子占据。因此,优化后的Co-MnO2电极在500 mg L−1 NaCl溶液中表现出优异的HCDI性能:高初始盐吸附容量(SAC)为83 mg g−1,快速盐吸附速率(SAR)为4.33 mg g−1 min−1,循环稳定性显著,循环150次后容量保留率为82%。实验表征证实了MnO结合强度的增强和锰溶解的抑制,验证了自旋态控制的有效性。这项工作建立了离子半径失配作为开发抗J-T扭曲电化学材料的通用设计原则,为海水淡化及其他领域的工程超耐用电极提供了新的见解。
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引用次数: 0
Environment-responsive phase transformation of Ni-modified cobalt phosphate aerogels for durable hydrogen evolution in freshwater and seawater 镍改性磷酸钴气凝胶在淡水和海水中持久析氢的环境响应相变研究
IF 9.8 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-06-01 Epub Date: 2026-02-26 DOI: 10.1016/j.desal.2026.120010
Younghun Kim , Sang-Hyun Kim , Jiseung Kim , Wonjun Lee , Hyun Jee Heo , In Hye Kwak , Vinayak G. Parale , Hyung-Ho Park
Non-precious 3d transition metal-based compounds are attractive electrocatalysts for the hydrogen evolution reaction (HER), but their structural instability under practical environments, particularly in seawater, remains a major challenge. Here, we report nickel modified cobalt phosphate (NCP) aerogels synthesized via a metal coordination-initiated sol-gel process, in which Ni incorporation governs environment-dependent reconstruction pathways. In freshwater, pristine cobalt phosphate undergoes surface oxidation toward crystalline oxyhydroxide species, whereas in seawater, Co(OH)2 phases dominate due to Cl-induced corrosion, resulting in compromised durability. Remarkably, Ni incorporation fundamentally alters these behaviors: in freshwater, it weakens the crystallinity of the CoOOH phase, and in seawater, it drives the formation of an amorphous CoOOH-rich matrix containing only minor Co(OH)2 domains. This Ni-induced disorder suppresses long-range crystalline hydroxide growth, stabilizes the surface against chloride attack, and facilitates charge transfer. The optimized NCP2.5 catalyst achieves low overpotentials in freshwater and seawater, respectively, along with Tafel slopes of 67.6 and 103.4 mV dec−1. It retains outstanding stability with only ~1% performance loss in freshwater after 100 h and ~ 8% in natural seawater after 100 h. These findings unveil a generalized design principle where dopant-induced amorphization guides environment-specific reconstruction pathways, providing design principles for robust and seawater-compatible hydrogen production.
非贵重的三维过渡金属基化合物是析氢反应(HER)的有吸引力的电催化剂,但其在实际环境下,特别是在海水中的结构不稳定性仍然是一个主要挑战。在这里,我们报道了通过金属配位引发的溶胶-凝胶过程合成的镍修饰磷酸钴(NCP)气凝胶,其中镍掺入控制环境依赖的重建途径。在淡水中,原始的磷酸钴表面氧化为结晶的氢氧化物,而在海水中,由于Cl−引起的腐蚀,Co(OH)2相占主导地位,导致耐久性降低。值得注意的是,Ni的加入从根本上改变了这些行为:在淡水中,它削弱了CoOOH相的结晶度,而在海水中,它驱动了只含有少量Co(OH)2结构域的无定形富CoOOH基体的形成。这种ni诱导的无序抑制了氢氧化物晶体的长程生长,稳定了表面对抗氯离子的攻击,并促进了电荷转移。优化后的NCP2.5催化剂在淡水和海水中分别实现了低过电位,Tafel斜率分别为67.6和103.4 mV dec−1。在淡水中,100 h后性能损失仅为~1%,在天然海水中,100 h后性能损失仅为~ 8%。这些发现揭示了一种通用的设计原则,即掺杂剂诱导的非晶化指导环境特异性重建途径,为稳健且与海水兼容的制氢提供了设计原则。
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引用次数: 0
A “solar basking cloth” evaporator constructed of Bi2OS2 hydrogel-melamine foam for efficient solar steam generation 一种由Bi2OS2水凝胶-三聚氰胺泡沫构成的“太阳能晒布”蒸发器,用于高效太阳能蒸汽产生
IF 9.8 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-06-01 Epub Date: 2026-03-03 DOI: 10.1016/j.desal.2026.120042
Yuding Yang , Die Lu , Yuhan Liu , Sihang Cheng , Cuimei Liu , Yangguang Li , Xiuli Wang
Solar-driven steam generation (SSG) technology, as a breakthrough solution to the global water crisis, not only establishes a green pathway for clean freshwater access but also pioneers an innovative paradigm for synergistic energy-environment governance. Currently, while significant academic progress has been made, overcoming bottlenecks in evaporation rate and energy conversion efficiency remains crucial for practical implementation. Here, this study constructs a bismuth oxide sulfide hydrogel-melamine foam evaporator (abbreviated as Bi2OS2 Gel-MF) featuring a three-dimensional multi-level water transport system via synthesizing novel Bi2OS2 nanosheets and drawing inspiration from traditional “solar basking cloth” structures. In this system, the hydrophilic MF framework acts as a “water transport artery” and continuously supplies water to the surface “evaporation fabric” (Bi2OS2 hydrogel), enabling rapid water transport and evaporation. Under standard solar irradiance, the Bi2OS2 Gel-MF achieves an evaporation rate of 3.30 kg m−2 h−1, demonstrating long-term sustainability and durability. This structure also exhibits excellent desalination performance and evaporation rates in practical seawater desalination, highlighting its potential applications in solar seawater desalination and photothermal water treatment.
太阳能蒸汽发电(SSG)技术作为解决全球水危机的突破性方案,不仅建立了清洁淡水获取的绿色途径,而且开创了能源-环境协同治理的创新范式。目前,虽然已经取得了重大的学术进展,但克服蒸发速率和能量转换效率方面的瓶颈仍然是实际实施的关键。本研究通过合成新型Bi2OS2纳米片,借鉴传统的“太阳能晒布”结构,构建了具有三维多层次水运系统的氧化铋硫化水凝胶-三聚氰胺泡沫蒸发器(简称Bi2OS2 Gel-MF)。在该系统中,亲水性MF框架作为“输水动脉”,不断向表面“蒸发织物”(Bi2OS2水凝胶)供水,实现快速的水运输和蒸发。在标准太阳辐照度下,Bi2OS2凝胶- mf的蒸发速率为3.30 kg m−2 h−1,具有长期可持续性和耐久性。该结构在实际海水淡化中也表现出优异的淡化性能和蒸发速率,突出了其在太阳能海水淡化和光热水处理中的潜在应用。
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引用次数: 0
Bioinspired 3D rolled evaporator with nanoconfined energy network for synergistic solar desalination and antibiotic degradation 生物启发的三维卷蒸发器与纳米限制的能源网络协同太阳能脱盐和抗生素降解
IF 9.8 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-06-01 Epub Date: 2026-02-19 DOI: 10.1016/j.desal.2026.119999
Xiaowen Cui , Xin Wang , Xiao Sun , Ting Wang , Yicheng Wang , Tinghui Wu , Haoyue Wu , Shengchen Wu , Yutong Liu , Junyi Tao , Yongqi Yang , Mengzhu Liu , Yongpeng Wang , Zhe Chen , Tao Jia
Addressing global freshwater scarcity requires advanced technologies that combine efficient desalination with the removal of emerging contaminants. Here, we report a banana tree-inspired three-dimensional (3D) rolled evaporator designed for high-performance solar desalination and simultaneous degradation of antibiotic pollutants. The evaporator is fabricated by anchoring a ZIF-67-derived, nanoconfined Co₃O₄/C composite onto a cotton gauze scaffold, with sodium alginate (SA) hydrogel acting as both a hydrophilic binder and an evaporation enthalpy regulator. The biomimetic 3D rolled geometry, mimicking the layered and curled structure of a banana tree stem, establishes a natural temperature gradient across its interlayer gaps, which facilitates continuous water replenishment and concentration-gradient-driven back diffusion of salt ions, enabling passive and self-regulated salt rejection without external energy input. The nanoconfined Co₃O₄/C composite not only exhibits excellent broadband photothermal conversion (average absorption of ~80.8%) but also serves as an efficient heterogeneous catalyst for peroxymonosulfate (PMS) activation. Under 1 sun irradiation, the evaporator achieves a high evaporation rate of 4.07 kg m−2 h−1 and an impressive energy efficiency of 94.01%, while maintaining stable performance in high-salinity brine (20 wt% NaCl) without salt accumulation. Moreover, the integrated system enables in-situ degradation of norfloxacin (NOR) via radical and non-radical pathways, reaching 90% removal within 120 min with minimal cobalt leaching. In summary, this work demonstrates a synergistic strategy that integrates a bioinspired three-dimensional architecture, a nanoconfined photothermal–catalytic energy network, and structure-regulated salt transport, enabling concurrent solar desalination and catalytic purification and offering a promising integrated solution for sustainable water treatment.
解决全球淡水短缺问题需要先进的技术,将有效的海水淡化与去除新出现的污染物结合起来。在这里,我们报道了一种受香蕉树启发的三维(3D)滚动蒸发器,该蒸发器设计用于高性能太阳能脱盐和同时降解抗生素污染物。蒸发器是通过将一种由zif -67衍生的纳米限制Co₃O₄/C复合材料锚定在棉纱支架上制成的,海藻酸钠(SA)水凝胶同时作为亲水性粘合剂和蒸发焓调节剂。仿生三维滚动几何形状,模仿香蕉树茎的分层和卷曲结构,在其层间间隙建立自然温度梯度,从而促进连续补水和浓度梯度驱动的盐离子反向扩散,实现被动和自我调节的排盐,而无需外部能量输入。纳米Co₃O₄/C复合材料不仅具有良好的宽带光热转化率(平均吸收率为~80.8%),而且是一种高效的过氧单硫酸盐(PMS)非均相活化催化剂。在1次太阳照射下,蒸发器的蒸发速率高达4.07 kg m−2 h−1,能量效率高达94.01%,同时在高盐度盐水(20 wt% NaCl)中保持稳定的性能,没有盐积累。此外,集成系统可以通过自由基和非自由基途径原位降解诺氟沙星(NOR),在120分钟内达到90%的去除率,并且钴浸出最少。总之,这项工作展示了一种协同策略,将生物启发的三维结构、纳米限制的光热催化能量网络和结构调节的盐运输结合在一起,实现了太阳能脱盐和催化净化的并行,并为可持续水处理提供了一个有前途的综合解决方案。
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引用次数: 0
Mass transfer study for the removal of copper ions from industrial wastewater using fluidized bed ion exchange reactor impingement with jet flow 射流冲击流化床离子交换反应器去除工业废水中铜离子的传质研究
IF 9.8 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-06-01 Epub Date: 2026-02-19 DOI: 10.1016/j.desal.2026.119998
S.E. Tafeh , H.A. Farag , G.H. Sedahmed , D.A. Elgayar
The removal of copper ions from industrial wastewater was investigated using a recirculating batch reactor consisting of a fluidized bed packed with a cation exchange resin and impinged by an axial turbulent submerged jet. The study systematically investigated the influence of key operating parameters, including the initial copper ion concentration, jet velocity, nozzle diameter, resin weight (g/L of solution), and the distance between the nozzle jet surface and the bottom of the reactor on the mass transfer performance. The experimental results indicated that the mass transfer rate increases with an increase in jet velocity, nozzle diameter, and resin weight dosage, while the mass transfer rate decreases with an increase in the initial copper ion concentration. Moreover, an enhancement in mass transfer rate was observed as the distance from the nozzle jet surface to the reactor bottom decreased, reaching a maximum at an optimal distance at 3–4 cm, beyond which the rate declined with further distance decrease. The results showed that using a fluidized jet reactor increased the rate of mass transfer up to 55 times compared to natural convection, achieving a copper ion removal efficiency of 96% with a mass transfer coefficient of 0.2 cm/s in just 16 min. The mass transfer data obtained from the experiments were analyzed using dimensionless analysis and mathematically correlated to develop a dimensionless equation suitable for design and scale-up. The present data fit the correlation: Sh=7105Re1.31Sc0.33 under the conditions 466.97 < Re < 4691.67, 1290.89 < Sc < 1416.53.
采用以阳离子交换树脂为填料,轴向湍流浸没射流冲击的流化床间歇式循环反应器对工业废水中的铜离子进行了脱除研究。研究系统考察了初始铜离子浓度、射流速度、喷嘴直径、树脂质量(g/L溶液)、喷嘴射流表面与反应器底部距离等关键操作参数对传质性能的影响。实验结果表明,传质速率随喷射速度、喷嘴直径和树脂质量投加量的增大而增大,随初始铜离子浓度的增大而减小。随着喷嘴射流表面到反应器底部的距离减小,传质速率增大,在3 ~ 4 cm处达到最大,超过该距离后传质速率随距离减小而减小。结果表明,与自然对流反应器相比,流态化射流反应器的传质速率提高了55倍,在16 min内以0.2 cm/s的传质系数实现了96%的铜离子脱除效率。对实验得到的传质数据进行了无因次分析和数学关联,建立了适合设计和放大的无因次方程。在466.97 < Re < 4691.67, 1290.89 < Sc <; 1416.53条件下,目前的数据符合相关性:Sh=7∗10−5Re1.31Sc0.33。
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引用次数: 0
Size-selective adsorption and multi-cycle treatment performance of hierarchical pitch-derived activated carbon for real textile effluent 分级沥青衍生活性炭对纺织废水的粒径选择性吸附及多循环处理性能
IF 9.8 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-06-01 Epub Date: 2026-02-12 DOI: 10.1016/j.desal.2026.119975
Yong Li , Dayeon Lee , Byeong-Chan Min , Tae Woon Kim , Jun Young Choi , Si-Hyeon Park , Chul-Woong Cho , Sung Wook Won
Industrial dye wastewater poses persistent environmental concerns; designing adsorbents with tailored porosity and high surface area is critical for efficient treatment. This work presents hierarchical pitch-derived activated carbon (P-PAC) synthesized via KOH activation, achieving an ultrahigh BET surface area (2614 m2/g) and a dual meso/microporous structure as verified by BET, XRD, FTIR, SEM-EDS, and XPS analyses. P-PAC exhibited superior adsorption capacities for Methylene Blue (867 mg/g), Acid Red 18 (505 mg/g), and Reactive Yellow 2 (417 mg/g), exceeding commercial activated carbons by more than two-fold. The exceptional performance arises from synergistic mechanisms including electrostatic attraction, π–π stacking by graphitic domains, and hydrogen bonding via oxygen functionalities. Crucially, the optimized hierarchical pore network enabled pronounced molecular sieving in competitive multi-dye systems (e.g., MB/RY2 selectivity factor = 15.1), which dictates the size-selective adsorption. P-PAC demonstrated superior multi-cycle treatment performance, maintaining high color removal efficiencies of 80–99% over 30 non-regenerative cycles when treating real textile effluent, which strongly validates its potential for long-term applications. This work establishes a performance–structure relationship that will guide the future design of high-efficiency adsorbents for large-scale industrial wastewater applications.
工业染料废水引起了持续的环境问题;设计具有定制孔隙度和高表面积的吸附剂对于有效处理至关重要。本文介绍了通过KOH活化合成的分层沥青衍生活性炭(P-PAC),通过BET、XRD、FTIR、SEM-EDS和XPS分析证实,该活性炭具有超高的BET表面积(2614 m2/g)和双介孔/微孔结构。P-PAC对亚甲基蓝(867 mg/g)、酸性红18 (505 mg/g)和活性黄2 (417 mg/g)的吸附能力均优于商用活性炭。这种特殊的性能源于静电吸引、石墨畴的π -π堆叠和氧官能团的氢键等协同机制。最重要的是,优化后的分层孔网络在竞争性多染料体系中实现了明显的分子筛分(例如,MB/RY2选择性因子= 15.1),这决定了尺寸选择性吸附。P-PAC表现出卓越的多循环处理性能,在处理实际纺织废水时,在30个非再生循环中保持80-99%的高去色效率,这有力地验证了其长期应用的潜力。这项工作建立了一种性能结构关系,将指导未来设计用于大规模工业废水应用的高效吸附剂。
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引用次数: 0
Surface-engineered PTFE-chitosan hybrid films for fluoride ion adsorption: A novel sorbent system 表面工程聚四氟乙烯-壳聚糖杂化膜:一种新型的氟离子吸附体系
IF 9.8 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-06-01 Epub Date: 2026-02-28 DOI: 10.1016/j.desal.2026.120033
Tejaswini A. Rathi , Vaishnavi Gomase , Neha Singh , D. Saravanan , Ravin Jugade
The recent research work presents a modified Poly tetrafluoroethylene (PTFE) cross-linked chitosan membrane (mPTFECs) as an effective adsorbent for the removal of fluoride (F) ions from aqueous systems. The batch adsorption process was statistically enhanced and validated using Response Surface Methodology. The maximum capacity of the mPTFECs for F was calculated to be 42.71 mg g−1, showing high affinity of mPTFECs for F. The data for adsorption in equilibrium were found to fit the Langmuir isotherm (R2 = 0.994) which indicates a monolayer adsorption on a homogeneous surface. Results of the kinetics study revealed that F adsorption was best explained by pseudo-second-order (R2 = 0.995). Thermodynamic studies indicate that F adsorption onto mPTFECs is spontaneous as well as exothermic and driven by enthalpy. The membrane's effectiveness was further tested on real water samples in actual conditions. Moreover, regeneration studies indicated that after five successive adsorption-desorption cycles, the membrane maintained significant adsorption performance, indicating its reusability and cost-effectiveness. The potential of mPTFECs as an effective and sustainable adsorbent for adsorption removal is highlighted in the study.
研究了一种改性聚四氟乙烯(PTFE)交联壳聚糖膜(mPTFECs)作为一种有效的吸附剂,用于去除水中的氟离子(F−)。采用响应面法对间歇吸附过程进行了统计增强和验证。mPTFECs对F−的最大容量为42.71 mg g−1,表明mPTFECs对F−具有较高的亲和力。平衡吸附数据符合Langmuir等温线(R2 = 0.994),表明在均匀表面上存在单层吸附。动力学研究结果表明,F−吸附最符合准二阶方程(R2 = 0.995)。热力学研究表明,氟离子在mPTFECs上的吸附是自发的,也是由焓驱动的放热吸附。在实际条件下对该膜的有效性进行了进一步的测试。此外,再生研究表明,在连续五次吸附-解吸循环后,膜保持了显著的吸附性能,表明其可重复使用和成本效益。该研究强调了mPTFECs作为一种有效和可持续的吸附去除剂的潜力。
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引用次数: 0
Highly efficient ammonium ion removal via a hybrid capacitive deionization platform with low-gap and structurally stable MIL-101(Fe)@cellulose nanocrystals 基于低间隙、结构稳定的MIL-101(Fe)@纤维素纳米晶的杂化电容去离子平台高效去除铵离子
IF 9.8 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-06-01 Epub Date: 2026-02-27 DOI: 10.1016/j.desal.2026.120002
Xuan Zhang , Chao Yan , Yuting Peng , Nannan Zhang , Jiaxin Gao , Minjie Shi , Jianming Pan
Metal-organic frameworks (MOFs) have surfaced as exceptionally promising porous materials, primarily because of their ability to form stable structures with remarkable properties. These frameworks possess numerous pores that enhance ion transport in capacitive deionization (CDI) applications. However, significant hurdles persist with MOFs, including a scarcity of active sites and complications related to water stability, which impede their broader usage. Additionally, the charge-discharge cycles that take place during operation can induce lattice distortions, a phenomenon associated with the Jahn-Teller effect that is intrinsic to MOF structures. To address this challenge, we have synthesized hybrid nanoparticles composed of MIL-101(Fe) and cellulose nanocrystals (CNCs), referred to as MCNCs, featuring a stable structure that integrates a π-conjugated framework characterized by extensive electron delocalization and a narrowed HOMO-LUMO gap. Additionally, the high density of active sites provided by CO groups promotes efficient redox reactions, enhancing the NH4+ capture capability. The produced MCNCs polymer demonstrates remarkable electro-adsorption properties and significant structural durability, achieving an impressive specific capacitance of 119.05 F g−1 at 0.5 A g−1. Leveraging the exceptional pseudocapacitive attributes of the MCNCs, we have engineered a hybrid capacitive deionization system that not only demonstrates an extraordinary ammonium removal capacity of 81.29 mg g−1 and a swift average removal rate of 3.75 mg g−1 min−1 but also retains 93.79% of its initial removal capacity for ammonium ions after 100 cycles, offering a fast, effective, and sustainable method for treating water.
金属有机框架(mof)作为一种非常有前途的多孔材料已经浮出水面,主要是因为它们能够形成具有卓越性能的稳定结构。这些框架具有许多孔隙,在电容去离子(CDI)应用中增强离子传输。然而,mof仍然存在一些重大障碍,包括活性位点的缺乏和与水稳定性相关的并发症,这些都阻碍了它们的广泛应用。此外,在操作过程中发生的充放电循环会引起晶格扭曲,这是一种与MOF结构固有的Jahn-Teller效应相关的现象。为了解决这一挑战,我们合成了由MIL-101(Fe)和纤维素纳米晶体(CNCs)组成的杂化纳米颗粒,简称mcnc,具有稳定的结构,集成了具有广泛电子离域和缩小HOMO-LUMO间隙的π共轭框架。此外,CO基团提供的高密度活性位点促进了有效的氧化还原反应,增强了NH4+的捕获能力。制备的mcnc聚合物具有显著的电吸附性能和显著的结构耐久性,在0.5 A g−1下达到了令人印象深刻的119.05 F g−1比电容。利用MCNCs独特的假电容特性,我们设计了一种混合电容去离子系统,不仅表现出81.29 mg g - 1的非凡铵离子去除率和3.75 mg g - 1 min - 1的快速平均去除率,而且在100次循环后仍保持其初始铵离子去除率的93.79%,提供了一种快速,有效和可持续的水处理方法。
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引用次数: 0
Crab pincer-inspired bionic porphyrin-based adsorbent to achieve capture-co-reduction of uranyl ions by dinitrogen chelation 蟹钳启发的仿生卟啉吸附剂,通过二氮螯合实现铀酰离子的捕获-共还原
IF 9.8 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-06-01 Epub Date: 2026-02-21 DOI: 10.1016/j.desal.2026.120003
Taotao Qiang , Chen Mi , Jie Xiong , Bing Shi , Sijie Yu , Fei Cheng , Longfang Ren
The hexavalent uranyl ions extracted from seawater cannot be directly used in nuclear energy, they must be further reduced to be tetravalent ones. However, the existing technologies nearly all focus on single adsorption or reduction, and there is very few studying on integrated adsorption-co-reduction method. Inspired by crab pincer, a novel adsorbent Ni-Por-1 was designed by using porphyrin as a framework and 2, 2′-bipyridine group as bidentate ligand, achieving adsorption-co-reduction of uranium from seawater. Ni-Por-1 has high photocurrent response and a narrow bandgap (1.39 eV), while the bidentate ligand can firmly capture uranyl ions. These endow it with excellent photocatalytic adsorption and in situ reduction properties. Under visible light irradiation, the adsorption equilibrium time of Ni-Por-1 is shortened to 60 min with an adsorption capacity of up to 249 mg g−1, simultaneously the reduction efficiency to uranium (VI) reaches 64%. Meantime, it shows excellent selective adsorption to uranium (Kd = 9.88 × 103 mL g−1) and antibacterial properties (99.8%). When used in natural seawater, the adsorption capacity of Ni-Por-1 reaches 4.52 mg g−1. This study realizes the integrated strategy of capture and in-situ photocatalytic reduction of uranyl ions, showing great strategic significance for the sustainable development of nuclear energy.
从海水中提取的六价铀酰离子不能直接用于核能,必须进一步还原为四价铀酰离子。然而,现有的技术几乎都集中在单一的吸附或还原上,对吸附-共还原一体化方法的研究很少。以蟹钳为灵感,以卟啉为骨架,以2,2′-联吡啶基为双齿配体,设计了一种新型吸附剂Ni-Por-1,实现了对海水中铀的吸附-共还原。Ni-Por-1具有高的光电流响应和窄的带隙(1.39 eV),而双齿配体可以牢固地捕获铀酰离子。这使其具有优异的光催化吸附和原位还原性能。在可见光照射下,ni - pir -1的吸附平衡时间缩短至60 min,吸附量高达249 mg g−1,同时对铀(VI)的还原效率达到64%。同时,对铀的选择性吸附(Kd = 9.88 × 103 mL g−1)和抗菌性能(99.8%)均表现优异。在天然海水中使用时,Ni-Por-1的吸附量达到4.52 mg g−1。本研究实现了铀酰离子的捕获与原位光催化还原一体化策略,对核能的可持续发展具有重要的战略意义。
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引用次数: 0
Spatial confinement on activated carbon enables uniformly dispersed FeOOH for stable capacitive defluoridation 空间限制上的活性炭使均匀分散的FeOOH稳定的电容除氟
IF 9.8 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-06-01 Epub Date: 2026-02-26 DOI: 10.1016/j.desal.2026.120027
Chulei Zhao , Dongxu Chen , Jiao Yin , Hui Zhu
This study addresses the challenges of active site agglomeration and insufficient cycling stability of iron oxyhydroxide (FeOOH) when used as an electrode material in capacitive deionization (CDI). A composite preparation strategy was proposed, which combines ultrasonic-assisted precursor uniform dispersion, urea-regulated crystallization, and hydrothermal in-situ growth. This approach successfully constructed a FeOOH@AC composite electrode featuring highly dispersed FeOOH nanoflowers on an activated carbon (AC) substrate. The spatial confinement effect of AC was utilized to effectively inhibit the agglomeration of FeOOH and alleviate volume expansion during cycling. Experimental results demonstrated that the prepared FeOOH@AC electrode exhibited a high salt adsorption capacity of 80.2 mg·g−1 during the CDI defluoridation process and retained over 90% of its capacity after 100 cycles, significantly outperforming most reported fluoride adsorbent materials. This work provides a material design strategy for constructing fluoride ion capture electrodes with high ion accessibility, rapid charge transfer, and long-term cycling stability.
本研究解决了氢氧化铁(FeOOH)作为电容去离子(CDI)电极材料时活性位点团聚和循环稳定性不足的问题。提出了超声辅助前驱体均匀分散、尿素调控结晶和水热原位生长相结合的复合制备策略。该方法在活性炭(AC)衬底上成功构建了具有高度分散的FeOOH纳米花的FeOOH@AC复合电极。利用活性炭的空间约束效应,有效抑制FeOOH的团聚,缓解循环过程中的体积膨胀。实验结果表明,制备的FeOOH@AC电极在CDI脱氟过程中具有80.2 mg·g−1的高盐吸附容量,并且在100次循环后仍保持90%以上的容量,显著优于大多数报道的氟吸附材料。这项工作为构建具有高离子可及性、快速电荷转移和长期循环稳定性的氟离子捕获电极提供了一种材料设计策略。
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引用次数: 0
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Desalination
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