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圖文摘要

成果簡(jiǎn)介

近日，張禮知教授課題組在Water Research上發(fā)表了題為“Renewable Energy Driven Electroreduction Nitrate to Ammonia and in-situ Ammonia Recovery via a Flow-Through Coupled Device”的研究論文(DIO: 10.1016/j.watres.2023.120256)，開發(fā)了用于連續(xù)電化學(xué)還原硝酸根產(chǎn)氨和原位回收氨的透過式耦合裝置。作者通過將透過式流動(dòng)電解池和中空疏水透氣膜單元進(jìn)行巧妙組合，實(shí)現(xiàn)了硝酸根到氨的快速轉(zhuǎn)換和同步高效回收氨。這項(xiàng)工作為硝酸根廢水資源化利用提供了一個(gè)可行方案。

全文速覽

本研究設(shè)計(jì)了一種可再生能源驅(qū)動(dòng)的新型透過式耦合裝置，旨在實(shí)現(xiàn)NO₃^?廢水資源化利用。該裝置的緊湊透過式流動(dòng)電解池能夠強(qiáng)化NO₃^?傳質(zhì)，有利于促進(jìn)NO₃^?還原到NH₃。同時(shí)，無需調(diào)節(jié)廢水pH和額外輸入能量，疏水透氣膜組件能夠快速原位回收NH₃。通過耦合高性能的Cl-Cu整體電極，該透過式耦合裝置能夠在50 mg NO₃^?-N L^?1廢水中持續(xù)穩(wěn)定運(yùn)行100 h，并實(shí)現(xiàn)420 μg h^?1 cm^?1的氨回收速率。在太陽能驅(qū)動(dòng)下，該裝置也能將工業(yè)NO₃^?廢水達(dá)標(biāo)處理并實(shí)現(xiàn)接近100%的NH₃回收效率，展現(xiàn)出巨大的工業(yè)應(yīng)用潛力。

引言

電化學(xué)還原處理硝酸根廢水并原位回收氨，有利于控制水體氮污染和實(shí)現(xiàn)氮循環(huán)利用。然而，該技術(shù)面臨巨大挑戰(zhàn)是缺乏連續(xù)還原NO₃^?和原位回收NH₃的集成式裝置。合理設(shè)計(jì)反應(yīng)器是應(yīng)對(duì)上述挑戰(zhàn)的關(guān)鍵。針對(duì)低濃度NO₃^?廢水中電化學(xué)轉(zhuǎn)換效率受限于傳質(zhì)的問題，優(yōu)化電解池中流體流動(dòng)模型被證實(shí)是有效措施。當(dāng)溶液透過式穿過（Flow-through）多孔電極時(shí)，其擴(kuò)散層距離將會(huì)從300 μm降低至1μm，這將顯著促進(jìn)NO₃^?傳質(zhì)。此外，采用緊湊的兩電極單池構(gòu)型能夠避免膜污染和降低內(nèi)阻，進(jìn)而降低能耗。

圖文導(dǎo)讀

Fig. 1. Scenario of renewable energy driven electrochemical nitrate reduction and in-situ NH₃ recovery. Copyright 2023, Elsevier Inc.

材料表征

Fig. 2. Structure characterizations. (a) Evolution of LSV curves during the electrochemical leaching process. (b) High-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) image of Cl-Cu. (c) STEM-EELS elemental mapping images of Cl-Cu. (d) Cu LMM Auger spectra of Cl-Cu, CuCl and Cu. (e) The normalized XANES spectra of the Cl-Cu, referenced Cu foil, CuCl and CuCl₂. (f) FT k³-weighted χ(k)-function of the EXAFS spectra at Cu K-edge. Copyright 2023, Elsevier Inc.

Cl-Cu電化學(xué)還原NO₃^?性能測(cè)試

Fig. 3. Electrocatalytic NITRR performance. (a) LSV curves of Cl-Cu and Cu with the presence or absence of NO₃^-. (b) The comparison of NH₃ yield and corresponding faradaic efficiency over Cl-Cu and Cu at different working potentials. (c) Comparisons of NH₃ yield, NO₃^- removal efficiency, selectivity and Faradaic efficiency between Cl-Cu and Cu. (d) The consecutive recycling tests at -0.65 V over Cl-Cu.  Copyright 2023, Elsevier Inc.

在三電極體系中初步評(píng)估Cl-Cu電化學(xué)還原NO₃^?產(chǎn)氨的性能。Cl修飾能夠顯著提升Cu的還原硝酸根的轉(zhuǎn)換率、選擇性、法拉第效率和產(chǎn)氨速率。同時(shí)，Cl-Cu在20次循環(huán)中也具有優(yōu)異的穩(wěn)定性。

機(jī)理分析

Fig. 4. Mechanism analysis. (a) Time-resolved ATR-FTIR spectra of Cl-Cu and Cu. (b) Schematic diagram of NO₃^- distribution on the surface of Cl-Cu and Cu. (c) In situ ATR-FTIR spectra of Cl-Cu and Cu at -0.65 V. (d) DMPO spin-trapping ESR spectra of Cl-Cu and Cu under argon atmosphere at -0.65 V. (e) The ELF of Cu (top) and Cl-Cu (below). (f) The NO₃^– adsorption configuration and charge density difference on Cu (top) and Cl-Cu (below), respectively. The yellow and blue iso-surfaces represent charge accumulation and depletion in the space, respectively. The iso-value is 0.0015 a.u. (g) The free-energy diagrams and pathways of H₂O dissociation on Cu and Cl-Cu. Copyright 2023, Elsevier Inc.

時(shí)間分辨的原位紅外光譜（ATR-FTIR）揭示Cl誘導(dǎo)產(chǎn)生的Cu^δ+能夠增強(qiáng)吸附NO₃^?，這將增加電極界面NO₃^?濃度，有利于促進(jìn)反應(yīng)動(dòng)力學(xué)。同時(shí)，原位電化學(xué)ATR-FTIR光譜，電子順磁波譜（ESR）和理論計(jì)算結(jié)果表明Cl和電極表面吸附H₂O間存在的氫鍵作用(Cl???H?OH)，能夠高效促進(jìn)H₂O解離產(chǎn)生活性物種氫自由基(H^*)用于NO₃^?還原。

基于Cl-Cu電極的透過式耦合裝置電化學(xué)還原硝酸根和原位回收氨性能測(cè)試

Fig. 5. Electrochemical nitrate conversion and in-situ ammonia recovery by the flow-through coupled device.(a) Optical image of the flow-through coupled device for synchronous electrocatalytic nitrate conversion and in-situ ammonia recovery. (b) Time-dependent product distribution using the flow-through coupled device. (c) IC chromatograms after treatment. (d) Long-term operation at 800 mA with a sustained NH₃ recovery. (e) XRD pattern of the recovered NH₄Cl(s) product. The inset shows the mass of NH₄Cl(s). (f) Time-dependent distribution of nitrogen species during the treatment of real industrial wastewater. (g) TN_removal efficiency and the concentration of generated NO₂^--N in the effluent during the continuous-flow operation of two tandem units for industrial wastewater treatment. Copyright 2023, Elsevier Inc.

經(jīng)濟(jì)價(jià)值分析

Fig. 6. Economic feasibility analysis of flow-through coupled device. (a) The expenditure analysis with or without the consideration of ammonia profits under multiple NO₃^?-N concentration from 50 to 300 mg L^?1. (b) Optical image of the solar-driven coupled device. (c) Time-dependent distribution of nitrogen species during the real wastewater treatment with the solar driven coupled device under real sunlight. (d) The evolution of current and recovered NH₄⁺concentration under real sunlight at different time. Copyright 2023 Elsevier Inc.

回收氨產(chǎn)生的收益能夠降低電化學(xué)技術(shù)廢水處理成本的21% ~ 33%。在太陽能驅(qū)動(dòng)下，該耦合裝置也能將工業(yè)NO₃^-廢水達(dá)標(biāo)處理和高效回收NH₃。

小結(jié)

課題組介紹

么艷彩 上海交通大學(xué)環(huán)境科學(xué)與工程學(xué)院副教授、博士生導(dǎo)師。研究方向?yàn)閱卧哟呋?、環(huán)境/能源電催化。以第一作者/通訊作者身份在Nature Catalysis、Journal of the American Chemical Society、Angewandte Chemie International Edition（2篇）、Water Research、Science Bulletin等期刊發(fā)表SCI論文12篇，部分研究成果被Chemical Review、Chemical Society Reviews、Technology Times、EurekAlert! 等國(guó)際科學(xué)媒體廣泛報(bào)道, 并多次被新華社、人民日?qǐng)?bào)、《人民日?qǐng)?bào)（海外版）》、人民網(wǎng)、科學(xué)網(wǎng)等多家國(guó)內(nèi)外主流媒體關(guān)注。申請(qǐng)發(fā)明專利6項(xiàng)，授權(quán)并成果轉(zhuǎn)化1項(xiàng)。撰寫英文專著1部。曾獲中科院“百篇優(yōu)博論文”和中科院院長(zhǎng)優(yōu)秀獎(jiǎng)、第7屆全國(guó)水處理與循環(huán)利用學(xué)術(shù)會(huì)議優(yōu)秀報(bào)告獎(jiǎng)。先后獲得國(guó)家自然科學(xué)基金、上海市科委面上項(xiàng)目、科技部重點(diǎn)研發(fā)計(jì)劃項(xiàng)目子課題、博士后站前特別資助、博士后面上資助等7項(xiàng)省部級(jí)項(xiàng)目資助?，F(xiàn)任Colloid and Surface Science編委。

https://doi.org/10.1016/j.watres.2023.120256