Efficient solar fuel production with a high-pressure CO_(2)-captured liquid feed  

电化学还原高压CO_(2)捕集溶液制太阳能燃料

作　　者：Kai Deng Ying Zhang Hao Feng Ning Liu Lushan Ma Jingjing Duan Yongjie Wang Dong Liu Qiang Li 邓楷;张莹;冯浩;刘宁;马路山;段静静;王永杰;刘东;李强(MIIT Key Laboratory of Thermal Control of Electronic Equipment,School of Energy and Power Engineering,Nanjing University of Science and Technology,Nanjing 210094,China;School of Science,Harbin Institute of Technology,Shenzhen 518055,China)

机构地区：[1]MIIT Key Laboratory of Thermal Control of Electronic Equipment,School of Energy and Power Engineering,Nanjing University of Science and Technology,Nanjing 210094,China [2]School of Science,Harbin Institute of Technology,Shenzhen 518055,China

出　　处：《Science Bulletin》2022年第14期1467-1476,M0004,共11页科学通报（英文版）

基　　金：supported by the National Natural Science Foundation of China(51888103,52006103,51976090,and 52006101);Scientific and Technological Innovation Project of Carbon Emission Peak and Carbon Neutrality of Jiangsu Province(BE2022024);Natural Science Foundation of Jiangsu Province(BK20200072,BK20200491,and BK20200500);China Postdoctoral Science Foundation(2020M681603)。

摘　　要：We demonstrated an efficient solar photovoltaic-powered electrochemical CO_(2) reduction device with a high-pressure CO_(2)-captured liquid feed.In an“air-to-barrel”picture,this device holds promise to avoid both high-temperature gaseous CO_(2) regeneration and high energy-cost gas product separation steps,while these steps are necessary for devices with a gaseous CO_(2) feed.To date,solar fuel production with a CO_(2)-saturated liquid feed suffers from high over-potential to suppress the hydrogen evolution reaction and consequently,low solar-to-chemical(STC)energy conversion efficiency.Here,we presented a distinct high-pressure operando strategy,i.e.,we took extra advantage of the high pressure in catalyst synthesis besides in the period of the CO_(2) reduction reaction(CO_(2)RR).The power of this strategy was demonstrated by a proof-of-concept device in which a representative copper catalyst was first synthesized in operando in a high-pressure(50 bar)CO_(2)-saturated KHCO3 solution,and then this high-pressure CO_(2)-captured liquid was converted to solar fuel using the operando synthesized Cu catalyst.This Cu catalyst achieved 95%CO_(2)RR selectivity at the recorded low potential of−0.3 V vs.RHE enabled by the combination of operando facet engineering and oxide derivation.Furthermore,this device achieved a record-high STC efficiency of 21.6%under outdoor illumination,superior to other CO_(2)-saturated liquid-fed devices,and compared favorably to gaseous CO_(2)-fed devices.本文提出了电化学还原高压CO_(2)捕集溶液制太阳能燃料的概念,其应用于CO_(2)捕集-转化集成系统时,可避免传统气相供给CO_(2)还原制燃料工艺中的高温条件CO_(2)气相再生步骤和高能耗气体产物分离步骤.目前,饱和CO_(2)溶液供给的太阳能制燃料系统需要较高的过电位来抑制析氢副反应,导致系统的太阳能-化学能转化效率低.本文提出了催化剂高压原位合成策略,在高压(压力50 bar)饱和KHCO_(3)溶液模拟的高压CO_(2)捕集溶液中合成铜催化剂,进一步将高压CO_(2)捕集溶液转化为燃料.该策略结合了原位晶面调控和氧化物衍生方法,使得铜催化剂在-0.3 V vs.RHE的低电位下实现了95%的CO_(2)还原选择性.此外,作者研制了太阳能光伏驱动的电化学还原高压CO_(2)捕集溶液制燃料原理样机,在户外光照条件下太阳能-化学能转化效率高达21.6%,超过了文献报道的饱和CO_(2)溶液供给的太阳能制燃料系统.

关 键 词：Solar fuel Carbon capture and utilization Operando nanocatalyst synthesis PHOTOELECTROCHEMICAL Energy conversion efficiency 

分 类 号：TK519[动力工程及工程热物理—热能工程] TQ426[化学工程]