Bridging laboratory research and practical utilization is of crucial importance for the development of green ammonia synthetic technologies. A decentralized photo-assisted electrochemical-based demonstrator has been p...Bridging laboratory research and practical utilization is of crucial importance for the development of green ammonia synthetic technologies. A decentralized photo-assisted electrochemical-based demonstrator has been proposed for green ammonia synthesis from renewable electricity, air and water, where well-known defect-laden WO_(3) is used as the working electrode, and a commercially available PV panel supplies renewable electricity. In this demonstrator, defect-laden WO_(3) exhibits the optimum electrochemical NH_(3) formation rate(4.51 × 10^(-12)mol s^(-1)cm^(-2)) in 0.1 M K_(2)SO_(4)in a photovoltaic electrochemical(PV-EC) system. A system-level energy and cost analysis was conducted to investigate its economic viability and a general evaluation tool for system performance and cost estimation was proposed. This advance enables the possibility of integrating the small-scale green ammonia demonstrator into a stand-alone farm system.展开更多
CONSPECTUS:The rapid increase in atmospheric CO_(2) concentration(∼420 ppm)has become one of the significant issues threatening human survival.As an effective measure to solve this major problem,renewable energy-powe...CONSPECTUS:The rapid increase in atmospheric CO_(2) concentration(∼420 ppm)has become one of the significant issues threatening human survival.As an effective measure to solve this major problem,renewable energy-powered catalytic CO_(2) conversion technologies have received vast attention in both academia and industry.Among these techniques,photothermal catalysis is a rising star with promising potential for CO_(2) conversion even under milder conditions.Indium oxide was among the first to be used in photothermal CO_(2) catalysis,and through its various forms,stoichiometries,and surface chemistry,it has become one of the most well-studied photothermal catalyst systems.Indium oxide is a highly tunable semiconductor for CO_(2) photocatalysis,which can be driven by both light photochemically and heat photothermally,thereby serving as an archetype for understanding how to optimize its performance for storing solar as chemical energy,through creative materials chemistry.展开更多
CO_(2) electroreduction (CO_(2) ER) using renewable energy is ideal for mitigating the greenhouse effect and closing the carbon cycle. Bicarbonate (HCO_(3)−) is most commonly employed as the electrolyte anion because ...CO_(2) electroreduction (CO_(2) ER) using renewable energy is ideal for mitigating the greenhouse effect and closing the carbon cycle. Bicarbonate (HCO_(3)−) is most commonly employed as the electrolyte anion because it is known to facilitate CO_(2) ER. However, its dynamics in the electric double layer remains obscure and requires more in-depth investigation. Herein, we investigate the refined reduction process of bicarbonate by employing in situ attenuated total reflectance surface-enhanced infrared absorption spectroscopy. By comparing the product distributions in Ar-saturated KCl and KHCO_(3) electrolytes, we confirmed CO production from HCO_(3)^(−) in the absence of an external CO_(2) source. Notably, in contrast to an electric compulsion, negatively charged HCO_(3)− anions were found to accumulate near the electrode surface. A reduction mechanism of HCO3− is proposed in that HCO3− is not adsorbed over a catalyst, but may be enriched near the electrode surface and converted to CO_(2) and react over Au and Cu electrodes. The dependence of the CO_(2) ER activity on the local HCO3− concentration was subsequently discovered, which was in turn dependent on the bulk HCO3− concentration and cathodic potential. In particular, the local HCO3− concentration was limited by the cathodic potential, leading to a plateau in the CO_(2) ER activity. The proposed mechanism provides insights into the interaction between the catalyst and the electrolyte in CO_(2) ER.展开更多
基金grateful to the Natural Sciences and Engineering Council of Canada for supportthe Nation Natural Science Foundation of China (NSFC 21878162,21872102)+4 种基金support of the NSFC(52102311)the Program for Guangdong Introducing Innovative and Entrepreneurial Teams (2019ZT08L101)the Special Fund for the Sci-tech Innovation Strategy of Guangdong Province(210629095860472)the Shenzhen Natural Science Foundation(GXWD20201231105722002-20200824163747001)the Shenzhen Key Laboratory of Eco-materials and Renewable Energy(ZDSYS20200922160400001)。
文摘Bridging laboratory research and practical utilization is of crucial importance for the development of green ammonia synthetic technologies. A decentralized photo-assisted electrochemical-based demonstrator has been proposed for green ammonia synthesis from renewable electricity, air and water, where well-known defect-laden WO_(3) is used as the working electrode, and a commercially available PV panel supplies renewable electricity. In this demonstrator, defect-laden WO_(3) exhibits the optimum electrochemical NH_(3) formation rate(4.51 × 10^(-12)mol s^(-1)cm^(-2)) in 0.1 M K_(2)SO_(4)in a photovoltaic electrochemical(PV-EC) system. A system-level energy and cost analysis was conducted to investigate its economic viability and a general evaluation tool for system performance and cost estimation was proposed. This advance enables the possibility of integrating the small-scale green ammonia demonstrator into a stand-alone farm system.
基金financially supported by the National Natural Science Foundation of China (51802208, 51920105005, 21902113, 51821002 and 91833303)the Natural Science Foundation of Jiangsu Province (BK20200101)the Collaborative Innovation Centre of Suzhou Nano Science & Technology, and the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD)the Natural Sciences and Engineering Council of Canada for support of this work
基金support of the National Key R&D Program of China(Grants No.2021YFF0502000)National Natural Science Foundation of China(Grants No.52102311)+4 种基金the Special Fund for the Sci-tech Innovation Strategy of Guangdong Province(Grants No.STKJ2021017)the Shenzhen Natural Science Foundation(Grants No.GXWD20201231105722002-20200824163747001)the Shenzhen Key Laboratory of Eco-materials and Renewable Energy(Grants No.ZDSYS20200922160400001)the University Development Fund(Grants No.UDF01001721)the U of T-ZJU Joint Seed Fund.
文摘CONSPECTUS:The rapid increase in atmospheric CO_(2) concentration(∼420 ppm)has become one of the significant issues threatening human survival.As an effective measure to solve this major problem,renewable energy-powered catalytic CO_(2) conversion technologies have received vast attention in both academia and industry.Among these techniques,photothermal catalysis is a rising star with promising potential for CO_(2) conversion even under milder conditions.Indium oxide was among the first to be used in photothermal CO_(2) catalysis,and through its various forms,stoichiometries,and surface chemistry,it has become one of the most well-studied photothermal catalyst systems.Indium oxide is a highly tunable semiconductor for CO_(2) photocatalysis,which can be driven by both light photochemically and heat photothermally,thereby serving as an archetype for understanding how to optimize its performance for storing solar as chemical energy,through creative materials chemistry.
基金This work is supported by the National Key Research and Development Program of China(2016YFB0600901)the National Natural Science Foundation of China(21525626,22038009,51861125104)the Program of Introducing Talents of Discipline to Universities(No.BP0618007)for financial support.
文摘CO_(2) electroreduction (CO_(2) ER) using renewable energy is ideal for mitigating the greenhouse effect and closing the carbon cycle. Bicarbonate (HCO_(3)−) is most commonly employed as the electrolyte anion because it is known to facilitate CO_(2) ER. However, its dynamics in the electric double layer remains obscure and requires more in-depth investigation. Herein, we investigate the refined reduction process of bicarbonate by employing in situ attenuated total reflectance surface-enhanced infrared absorption spectroscopy. By comparing the product distributions in Ar-saturated KCl and KHCO_(3) electrolytes, we confirmed CO production from HCO_(3)^(−) in the absence of an external CO_(2) source. Notably, in contrast to an electric compulsion, negatively charged HCO_(3)− anions were found to accumulate near the electrode surface. A reduction mechanism of HCO3− is proposed in that HCO3− is not adsorbed over a catalyst, but may be enriched near the electrode surface and converted to CO_(2) and react over Au and Cu electrodes. The dependence of the CO_(2) ER activity on the local HCO3− concentration was subsequently discovered, which was in turn dependent on the bulk HCO3− concentration and cathodic potential. In particular, the local HCO3− concentration was limited by the cathodic potential, leading to a plateau in the CO_(2) ER activity. The proposed mechanism provides insights into the interaction between the catalyst and the electrolyte in CO_(2) ER.
