高效渗透驱动的绿色氢气生产！
氢气作为一种清洁能源载体，已成为实现电力行业去碳化和迈向更可持续未来的一种前景广阔的解决方案。然而，由于氢的生产严重依赖化石燃料，因此迫切需要优先从可再生资源中获取绿色氢，理想情况下无需任何额外的能源输入。
鉴于此，复旦大学孔彪教授和赵东元院士、江雷院士合作利用海水和淡水之间的渗透能直接生成氢气。通过串联高性能离子交换膜和电催化电极，该设计可收集渗透能并驱动制氢。值得注意的是，在人工盐度梯度条件下，该集成装置在超过12天的时间内显示出超过300 l m
-2h
-1的稳定碱性氢进化率。该研究为利用可再生资源制氢提供了一条可行的途径。相关研究成果以题为“Efficient osmosis-powered production of green hydrogen”发表在《Nature Sustainability》。
【装置设计】
在双路径超组装策略中，有两条不同的路径。在路径1中，植酸（PA）分子经过蒸发诱导组装，与热解ZIF-8得到的碳框架(CF)表面的氮原子结合。这种复合物通过流体导向组装进一步组装到阳极氧化铝（AAO）基底上，从而形成PA-CF/AAO混合膜。在路径2中，通过调节反应体系的pH值，选择性地将Pd原子组装到CF表面的纳米团簇中。生成的Pd-CF复合物随后与Nafion溶液混合，沉积到玻璃碳电极(GCE)表面，形成Pd-CF/GCE混合电极。PA-CF/AAO混合膜和Pd-CF/GCE混合电极这两个组件最终被集成在同一个电路中，从而建立了一个以渗透为动力的制氢装置（图1）。
图 1. 渗透驱动制氢集成装置的超组装
【表征】
PA-CF/AAO杂化膜具有不对称结构，可以根据需要调节PA-CF积累层的厚度（图2a-d）。Pd-CF/GCE混合电极的活性成分来自Pd-CF，通过在合成阶段调节pH值，可以在CF表面获得三种不同形式的Pd原子组装：单原子、纳米团簇和微小纳米颗粒（图2e）。当pH值从1.4逐渐升高到4.4时，CF表面会发生转变，从缺乏可辨认的金属颗粒转变为大小约为0.9纳米的纳米团簇，并进一步演变为微小的纳米颗粒（图2f-i）。经像差校正的高角度环形暗场扫描透射电子显微镜（AC HAADF-STEM）图像显示了亚纳米钯，PdI-CF 表面的孤立亮点与单个钯原子相对应，而 PdII-CF 表面的亮点则微弱地聚集成星云状纳米团簇（图 2g、k）。此外，在PdI-CF中只检测到与Pd
2+相对应的结合能峰，而在PdII-CF和PdIII-CF/PdIV-CF中则观察到与Pd
0相关的微弱（或明显）峰（图2l-o）。这些结果表明，Pd原子在CF上的组装形式随pH值的变化而变化。
图 2. 杂化膜和电极的表征
【膜性能】
在不同浓度的中性氯化钾电解质下获得的I-V曲线证明了PA-CF/AAO混合膜的线性欧姆行为。PA-CF/AAO混合膜的离子跨膜传输受表面电荷的影响（图3a），此外，PA-CF/AAO混合膜强大的阳离子选择性，促进了阳离子从PA-CF侧优先迁移到AAO侧（图3b）。同时，PA-CF/AAO混合膜表现出极佳的稳定性（图3c）。图3d结果凸显了该膜在不同盐度梯度下具有出色的阳离子选择性和能量转换效率。PA-CF/AAO混合膜在人工海水和淡水梯度条件下显示出近似184 mV的开路电压（V
OC）和25 μA的短路电流（ISC）（图3e）。电流密度随着外加电阻的增大而逐渐减小，最大输出功率密度达到28.3 Wm
-2，超过了纯AAO、ZIF-8/AAO、CF/AAO、商用Nafion-117膜以及目前报道的最先进的纳米流体装置（图3f、g）。膜厚度与发电量之间的关系结果显示极化效应与电阻耗散之间存在权衡（图3h）。此外，PA-CF/AAO混合膜在很宽的pH值范围和低温条件下都表现出稳定而强大的渗透能量收集性能，从而将其适用性扩展到各种应用场景（图3i、j）。
图 3. 杂化膜的离子传输和渗透能转换
【混合电极的性能】
PdII-CF在碱性溶液中的表现优于最近报道的大多数先进的钯基氢进化电催化剂（图4a）。随着过电位的增加，PdII-CF的氢气进化质量活性极化曲线呈现出最显著的下降（图4b）。在约50 mV的过电位下，PdII-CF的质量活度为1.24 A mg
-1，分别是商用Pt-C（0.09 A mg
-1）和Pd-C（0.02 A mg
-1）的约13倍和51倍（图4c）。集成设备的输出电压与人工海水-淡水系统中串联的配置表现出精确的线性相关性（图4d-f）。稳定性测试进一步表明，渗透驱动端口可以保持稳定运行超过 12 天（图 4g）。集成设备成功运行后，渗透动力端口不断将海水和淡水之间的渗透能转化为电能。同时，氢气发生口进行电催化水分解反应，导致电极表面沉淀出稳定的气泡流（图4h）。采用排水法收集集成装置运行过程中产生的氢气。结果表明，制氢口的氢气产率在短时间内可以达到~316 l m
−2h
−1（图4i）。此外，超过300 l m
−2h
−1的产率可以持续长达12天，证明了氢气生产的显着稳定性和效率（图4j）。据估计，大型集成装置可节省约38.08 或者44 kWh。与仅使用Pt-C/GCE或Pd-C/GCE析氢电极的传统电催化水分解装置相比，每产生一公斤氢气可节省02 kWh的电量（图4k）。这凸显了智能灵敏设备在绿色氢气生产方面的巨大潜力。
图 4. 混合电极和集成装置的性能评估
【不对称离子传输】
基于泊松-能斯特-普朗克 (PNP) 方程的 COMSOL 模拟进一步验证了不对称电荷分布和通道结构对杂化膜离子选择性的影响，揭示了与 Cl
− 相比，通道中传输的 K
+ 浓度更高（图5a）。Pd 的离子态根据溶液的 pH 值呈现不同的形式（图 5b）。图5c展示了仿生集成装置的工作机制。
图 5. 离子传输机制、Pd 原子组装调节和集成装置的操作
【总结】
本文在高性能离子交换膜和电催化电极超组装制备的集成装置中实现了渗透驱动的直接制氢。由于离子交换膜具有独特的非对称通道结构和Janus异质电荷分布特性，海水与淡水交界处的渗透发电端口在室温下工作时，其最大输出功率比现有的商业同类产品高出近六倍。同时，由于电极表面活性金属的亚纳米结构提供了丰富的超多活性位点，该装置制氢端口在碱性电解质中的氢气进化质量活性比同类产品高出约51倍，并能保持50mV的过电位。稳定性测试表明，在最佳条件下，微型集成装置能以超过300 l m
-2h
-1的速率连续制氢12天以上。与商用电催化分水装置相比，估计该集成装置可节省约40 kWh kg
-1的制氢耗电量，与标准火力发电（耗煤量约为330 g kWh
-1）相比，可减少约26 kg的二氧化碳排放量。这项工作有望推动进一步的实验和理论研究，以实现渗透制氢技术的实际应用。
【简介】
孔彪，国家重点研发计划首席科学家，入选国家高层次人才青年项目，上海市高层次人才特聘专家，复旦大学研究员、博士生导师，复旦大学山东研究院常务副院长，国家工程实验室副主任，国际Frontiers系列刊物副主编，《中国化学快报》Chinese Chemical Letters（CCL）编委，Mater Today Sustainability期刊编委以及Nano Research期刊青年编委（Young Star Editor）。
来源：高分子科学前沿
声明：仅代表个人观点，水平有限，如有不科学之处，请在下方留言指正！
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255, 255, .65);--weui-FG-1: rgba(255, 255, 255, .55);--weui-FG-2: rgba(255, 255, 255, .35);--weui-FG-3: rgba(255, 255, 255, .1);--weui-FG-4: rgba(255, 255, 255, .15);--weui-FG-5: rgba(255, 255, 255, .1);--weui-RED: #fa5151;--weui-ORANGERED: #ff6146;--weui-ORANGE: #c87d2f;--weui-YELLOW: #cc9c00;--weui-GREEN: #74a800;--weui-LIGHTGREEN: #3eb575;--weui-BRAND: #07c160;--weui-BLUE: #10aeff;--weui-INDIGO: #1196ff;--weui-PURPLE: #8183ff;--weui-WHITE: rgba(255, 255, 255, .8);--weui-LINK: #7d90a9;--weui-TEXTGREEN: #259c5c;--weui-FG: #fff;--weui-BG: #000;--weui-TAG-TEXT-RED: rgba(250, 81, 81, .6);--weui-TAG-BACKGROUND-RED: rgba(250, 81, 81, .1);--weui-TAG-TEXT-ORANGE: rgba(250, 157, 59, .6);--weui-TAG-BACKGROUND-ORANGE: rgba(250, 157, 59, .1);--weui-TAG-TEXT-GREEN: rgba(6, 174, 86, .6);--weui-TAG-BACKGROUND-GREEN: rgba(6, 174, 86, .1);--weui-TAG-TEXT-BLUE: rgba(16, 174, 255, .6);--weui-TAG-BACKGROUND-BLUE: rgba(16, 174, 255, .1);--weui-TAG-TEXT-BLACK: rgba(255, 255, 255, .5);--weui-TAG-BACKGROUND-BLACK: rgba(255, 255, 255, .05)}}@media screen and (min-width:1024px){body:not(.pages_skin_pc) .wx-root,body:not(.pages_skin_pc) body{--appmsgExtra-BG: #F7F7F7}}@media screen and (min-width:1024px){body:not(.pages_skin_pc) .wx-root[data-weui-theme=dark],body:not(.pages_skin_pc) body[data-weui-theme=dark]{--weui-BG-0: #111;--weui-BG-1: #1e1e1e;--weui-BG-2: #191919;--weui-BG-3: #202020;--weui-BG-4: #404040;--weui-BG-5: #2c2c2c;--weui-FG-0: rgba(255, 255, 255, .8);--weui-FG-HALF: rgba(255, 255, 255, .6);--weui-FG-1: rgba(255, 255, 255, .5);--weui-FG-2: rgba(255, 255, 255, .3);--weui-FG-3: rgba(255, 255, 255, .1);--weui-FG-4: rgba(255, 255, 255, .15);--weui-FG-5: rgba(255, 255, 255, .1);--weui-RED: #fa5151;--weui-ORANGERED: #ff6146;--weui-ORANGE: #c87d2f;--weui-YELLOW: #cc9c00;--weui-GREEN: #74a800;--weui-LIGHTGREEN: #3eb575;--weui-BRAND: #07c160;--weui-BLUE: #10aeff;--weui-INDIGO: #1196ff;--weui-PURPLE: #8183ff;--weui-WHITE: rgba(255, 255, 255, .8);--weui-LINK: #7d90a9;--weui-TEXTGREEN: #259c5c;--weui-FG: #fff;--weui-BG: #000;--weui-TAG-TEXT-RED: rgba(250, 81, 81, .6);--weui-TAG-BACKGROUND-RED: rgba(250, 81, 81, .1);--weui-TAG-TEXT-ORANGE: rgba(250, 157, 59, .6);--weui-TAG-BACKGROUND-ORANGE: rgba(250, 157, 59, .1);--weui-TAG-TEXT-GREEN: rgba(6, 174, 86, .6);--weui-TAG-BACKGROUND-GREEN: rgba(6, 174, 86, .1);--weui-TAG-TEXT-BLUE: rgba(16, 174, 255, .6);--weui-TAG-BACKGROUND-BLUE: rgba(16, 174, 255, .1);--weui-TAG-TEXT-BLACK: rgba(255, 255, 255, .5);--weui-TAG-BACKGROUND-BLACK: rgba(255, 255, 255, .05)}}@media screen and (min-width:1024px){body:not(.pages_skin_pc) .wx-root[data-weui-theme=dark],body:not(.pages_skin_pc) body[data-weui-theme=dark]{--appmsgExtra-BG: #121212}}@media screen and (min-width:1024px){body:not(.pages_skin_pc)body:not(.pages_skin_pc){background:var(--weui-BG-2)}}@media screen and (min-width:1024px) and (prefers-color-scheme:dark){body:not(.pages_skin_pc) .wx-root[data-weui-mode=care]:not([data-weui-theme=light]),body:not(.pages_skin_pc) body[data-weui-mode=care]:not([data-weui-theme=light]){--weui-BG-0: #111;--weui-BG-1: #1e1e1e;--weui-BG-2: #191919;--weui-BG-3: #202020;--weui-BG-4: #404040;--weui-BG-5: #2c2c2c;--weui-FG-0: rgba(255, 255, 255, .85);--weui-FG-HALF: rgba(255, 255, 255, .65);--weui-FG-1: rgba(255, 255, 255, .55);--weui-FG-2: rgba(255, 255, 255, .35);--weui-FG-3: rgba(255, 255, 255, .1);--weui-FG-4: rgba(255, 255, 255, .15);--weui-FG-5: rgba(255, 255, 255, .1);--weui-RED: #fa5151;--weui-ORANGERED: #ff6146;--weui-ORANGE: #c87d2f;--weui-YELLOW: #cc9c00;--weui-GREEN: #74a800;--weui-LIGHTGREEN: #3eb575;--weui-BRAND: #07c160;--weui-BLUE: #10aeff;--weui-INDIGO: #1196ff;--weui-PURPLE: #8183ff;--weui-WHITE: rgba(255, 255, 255, .8);--weui-LINK: #7d90a9;--weui-TEXTGREEN: #259c5c;--weui-FG: #fff;--weui-BG: #000;--weui-TAG-TEXT-RED: rgba(250, 81, 81, .6);--weui-TAG-BACKGROUND-RED: rgba(250, 81, 81, .1);--weui-TAG-TEXT-ORANGE: rgba(250, 157, 59, .6);--weui-TAG-BACKGROUND-ORANGE: rgba(250, 157, 59, .1);--weui-TAG-TEXT-GREEN: rgba(6, 174, 86, .6);--weui-TAG-BACKGROUND-GREEN: rgba(6, 174, 86, .1);--weui-TAG-TEXT-BLUE: rgba(16, 174, 255, .6);--weui-TAG-BACKGROUND-BLUE: rgba(16, 174, 255, .1);--weui-TAG-TEXT-BLACK: rgba(255, 255, 255, .5);--weui-TAG-BACKGROUND-BLACK: rgba(255, 255, 255, .05)}}@media screen and (min-width:1024px) and (prefers-color-scheme:dark){body:not(.pages_skin_pc) .wx-root:not([data-weui-theme=light]),body:not(.pages_skin_pc) body:not([data-weui-theme=light]){--weui-BG-0: #111;--weui-BG-1: #1e1e1e;--weui-BG-2: #191919;--weui-BG-3: #202020;--weui-BG-4: #404040;--weui-BG-5: #2c2c2c;--weui-FG-0: rgba(255, 255, 255, .8);--weui-FG-HALF: rgba(255, 255, 255, .6);--weui-FG-1: rgba(255, 255, 255, .5);--weui-FG-2: rgba(255, 255, 255, .3);--weui-FG-3: rgba(255, 255, 255, .1);--weui-FG-4: rgba(255, 255, 255, .15);--weui-FG-5: rgba(255, 255, 255, .1);--weui-RED: #fa5151;--weui-ORANGERED: #ff6146;--weui-ORANGE: #c87d2f;--weui-YELLOW: #cc9c00;--weui-GREEN: #74a800;--weui-LIGHTGREEN: #3eb575;--weui-BRAND: #07c160;--weui-BLUE: #10aeff;--weui-INDIGO: #1196ff;--weui-PURPLE: #8183ff;--weui-WHITE: rgba(255, 255, 255, .8);--weui-LINK: #7d90a9;--weui-TEXTGREEN: #259c5c;--weui-FG: #fff;--weui-BG: #000;--weui-TAG-TEXT-RED: rgba(250, 81, 81, .6);--weui-TAG-BACKGROUND-RED: rgba(250, 81, 81, .1);--weui-TAG-TEXT-ORANGE: rgba(250, 157, 59, .6);--weui-TAG-BACKGROUND-ORANGE: rgba(250, 157, 59, .1);--weui-TAG-TEXT-GREEN: rgba(6, 174, 86, .6);--weui-TAG-BACKGROUND-GREEN: rgba(6, 174, 86, .1);--weui-TAG-TEXT-BLUE: rgba(16, 174, 255, .6);--weui-TAG-BACKGROUND-BLUE: rgba(16, 174, 255, .1);--weui-TAG-TEXT-BLACK: rgba(255, 255, 255, .5);--weui-TAG-BACKGROUND-BLACK: rgba(255, 255, 255, .05)}}@media screen and (min-width:1024px) and (prefers-color-scheme:dark){body:not(.pages_skin_pc) .wx-root:not([data-weui-theme=light]),body:not(.pages_skin_pc) body:not([data-weui-theme=light]){--appmsgExtra-BG: #121212}}@media(prefers-color-scheme:dark){body:not([data-weui-theme=light]).my_comment_empty_data{background-color:#111}}body,.wx-root{--weui-BG-6: rgba(0, 0, 0, .05);--weui-ACTIVE-MASK: rgba(0, 0, 0, .05)}body,.wx-root{--weui-REDORANGE: #ff6146;--weui-BG-0: #ededed;--weui-BG-1: #f7f7f7;--weui-BG-2: #fff;--weui-BG-3: #f7f7f7;--weui-BG-4: #4c4c4c;--weui-BG-5: #fff;--weui-FG-0: rgba(0, 0, 0, .9);--weui-FG-HALF: rgba(0, 0, 0, .9);--weui-FG-1: rgba(0, 0, 0, .55);--weui-FG-2: rgba(0, 0, 0, .3);--weui-FG-3: rgba(0, 0, 0, .1);--weui-FG-4: rgba(0, 0, 0, .15);--weui-FG-5: rgba(0, 0, 0, .05);--weui-RED: #fa5151;--weui-ORANGERED: #ff6146;--weui-ORANGE: #fa9d3b;--weui-YELLOW: #ffc300;--weui-GREEN: #91d300;--weui-LIGHTGREEN: #95ec69;--weui-BRAND: #07c160;--weui-BLUE: #10aeff;--weui-INDIGO: #1485ee;--weui-PURPLE: #6467f0;--weui-WHITE: #fff;--weui-LINK: #576b95;--weui-TEXTGREEN: #06ae56;--weui-FG: #000;--weui-BG: #fff;--weui-TAG-TEXT-RED: rgba(250, 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#fff;--weui-LINK: #576b95;--weui-TEXTGREEN: #06ae56;--weui-FG: #000;--weui-BG: #fff;--weui-TAG-TEXT-RED: rgba(250, 81, 81, .6);--weui-TAG-BACKGROUND-RED: rgba(250, 81, 81, .1);--weui-TAG-TEXT-ORANGE: #fa9d3b;--weui-TAG-BACKGROUND-ORANGE: rgba(250, 157, 59, .1);--weui-TAG-TEXT-GREEN: #06ae56;--weui-TAG-BACKGROUND-GREEN: rgba(6, 174, 86, .1);--weui-TAG-TEXT-BLUE: #10aeff;--weui-TAG-BACKGROUND-BLUE: rgba(16, 174, 255, .1);--weui-TAG-TEXT-BLACK: rgba(0, 0, 0, .5);--weui-TAG-BACKGROUND-BLACK: rgba(0, 0, 0, .05)}.wx-root,body{--weui-BTN-ACTIVE-MASK: rgba(0, 0, 0, .1)}.wx-root,body{--weui-BTN-DEFAULT-ACTIVE-BG: #e6e6e6}.wx-root,body{--weui-DIALOG-LINE-COLOR: rgba(0, 0, 0, .1)}.wx-root,body{--weui-BG-COLOR-ACTIVE: #ececec}@media(prefers-color-scheme:dark){.wx-root:not([data-weui-theme=light]),body:not([data-weui-theme=light]){--weui-BTN-ACTIVE-MASK: rgba(255, 255, 255, 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59, .6);--weui-TAG-BACKGROUND-ORANGE: rgba(250, 157, 59, .1);--weui-TAG-TEXT-GREEN: rgba(6, 174, 86, .6);--weui-TAG-BACKGROUND-GREEN: rgba(6, 174, 86, .1);--weui-TAG-TEXT-BLUE: rgba(16, 174, 255, .6);--weui-TAG-BACKGROUND-BLUE: rgba(16, 174, 255, .1);--weui-TAG-TEXT-BLACK: rgba(255, 255, 255, .5);--weui-TAG-BACKGROUND-BLACK: rgba(255, 255, 255, .05)}}@media(prefers-color-scheme:dark){.wx-root:not([data-weui-theme=light]),body:not([data-weui-theme=light]){--discussInput-BG: rgba(255, 255, 255, .03)}}@media(prefers-color-scheme:dark){.wx-root:not([data-weui-theme=light]),body:not([data-weui-theme=light]){--nickName-FG: #959595}}@media(prefers-color-scheme:dark){.wx-root:not([data-weui-theme=light]),body:not([data-weui-theme=light]){--weui-BG-0: #111;--weui-BG-1: #1e1e1e;--weui-BG-2: #191919;--weui-BG-3: #202020;--weui-BG-4: #404040;--weui-BG-5: #2c2c2c;--weui-FG-0: rgba(255, 255, 255, .8);--weui-FG-HALF: rgba(255, 255, 255, .6);--weui-FG-1: rgba(255, 255, 255, .5);--weui-FG-2: rgba(255, 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