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| 1 | CeO_(2)担载Cu纳米粒子电催化CO_(2)还原产乙烯:CeO_(2)不同暴露晶面对催化性能的影响显示文摘化石燃料在未来几十年仍然是主要的能量来源,但是这种不可再生资源的燃烧释放出大量的CO_(2)(主要的温室气体),空气中CO_(2)的浓度每年仍然持续增加。使用间歇性可再生能源转化的电能驱动电化学CO_(2)还原生成高附加值产品为其减排提供了一种有前景、CO_(2)“零排放”的方法。本文通过利用Cu和不同形状的CeO_(2)纳米晶之间的相互作用,即分别暴露(100)、(110)、(111)晶面的立方体、棒状和八面体CeO_(2),实现了对电化学CO_(2)还原产乙烯的有效调控。研究发现,电化学CO_(2)还原的选择性和活性与CeO_(2)暴露的晶面密切相关,生成乙烯的法拉第效率和偏电流密度在1.00到1.15 V(相对于可逆氢电极)的施加电势范围内呈现出Cu/CeO_(2)(111) | 楚森林 李欣 Alex W.Robertson 孙振宇 | 2021 | 物理化学学报2021，37，5： | 9 |
| 2 | 超细氧化铜纳米颗粒修饰二维金属有机框架协同增强二氧化碳电化学还原生成乙烯显示文摘为了促进CO_(2)电化学还原(ECR)制备燃料和高值化学品,开发高活性、低成本和高选择性催化剂至关重要.本文通过简单的溶剂热法一步合成超细氧化铜(CuO)纳米颗粒修饰的二维Cu基金属有机框架(CuO/Cu-MOF)复合催化剂.并采用X射线衍射、X射线光电子能谱、傅里叶变换红外光谱、高角环形暗场像-扫描透射电镜、N_(2)吸附/脱附、元素分析谱、CO_(2)吸附等方法进行表征,对CuO/Cu-MOF复合材料的组成、形貌和孔结构等进行了系统研究.结果表明,超细CuO纳米粒子的尺寸为1.4到3.3 nm,均匀修饰在二维Cu-BDC MOF表面.由于其结构中丰富的孔道结构,CuO/Cu-MOF在常压下的CO_(2)吸附量可达5.0 mg_(CO2) g_(cat).^(–1),明显优于商业CuO纳米颗粒.进一步在H型电解池、0.1 mol/L KHCO_(3)电解质溶液中研究了CuO/Cu-MOF的ECR性能;结果表明,在CO_(2)饱和的0.1 mol/L KHCO_(3)电解质溶液中,反应产物包括CO,H_(2),HCOOH和C_(2)H_(4).在-1.0至-1.2 V(相对于可逆氢电极,下同)电势范围内,ECR占主导地位;生成C_(2)H_(4)的起始电位为-0.85 V,在-0.9至-1.2 V电势范围内,C_(2)H_(4)是主要产物;电势高于-0.9 V时,CO和HCOOH是主要产物;电势低于-0.9 V时,开始生成CH_(4),且其含量随过电势增加而增加.通过改变材料合成时的前驱体配比、配体种类和反应温度等可调节CuO/Cu-MOF催化剂对ECR产物的活性和选择性,当对苯二甲酸:硝酸铜摩尔比为3:1、温度为100°C时,制得的CuO/Cu-MOF可在-1.1 V电势下将CO_(2)还原为C_(2)H_(4),其法拉第效率可达50.0%,显著优于许多文献报道的Cu基电催化剂以及所合成的纯Cu-MOF和纯CuO,其在相同电解条件下生成C_(2)H_(4)的法拉第效率分别为37.6%和25.5%.此外,生成C_(2)H_(4)的几何分电流密度约为7.0 mA cm^(-2),生成速率为21.0μmol mg_(cat).^(–1) h^(–1),阴极能量效率达到27.7%.催化剂的稳定性测试结果表明,在连续电解10 h后,C_(2)H_(4)的法拉第效率仍保持在45.0%以上.进一步的机理研究表明,CuO/Cu-MOF复合材料中二维金属铜有机框架主体和超细CuO纳米颗粒在ECR反应过程中可协同实现对CO_(2)的吸附和活化,促进C-C耦合,从而高选择性生成C_(2)H_(4).本文为提高ECR生成C_(2)H_(4)的选择性和活性提供了有效策略. | 王琳琳 李欣 郝磊端 洪崧 Alex W.Robertson 孙振宇 | 2022 | Chinese Journal of Catalysis2022，43，4： | 4 |
| 3 | Single atom and defect engineering of CuO for efficient electrochemical reduction of CO_(2) to C_(2)H_(4)显示文摘Electrochemical CO_(2) transformation to high‐value ethylene(C_(2)H_(4))at high currents and efficiencies is desired and yet remains a grand challenge.We show for the first time that coupling single Sb atoms and oxygen vacancies of CuO enable synergistic electrocatalytic reduction of CO_(2) to C_(2)H_(4) at low overpotentials.Highly dispersed Sb atoms occupying metal substitutional sites of CuO are synthesized under mild conditions.The overall CO_(2) reduction faradaic efficiency(FE)reaches 89.3±1.1%with an FE toward C_(2)H_(4) exceeding 58.4%at a high‐current density of 500 mA/cm^(2).Addition of the p‐block metal is found to induce transformation of CuO from flakes to nanoribbons rich in nanoholes and oxygen vacancies,greatly enhancing CO_(2) adsorption and activation while suppressing hydrogen evolution.Further density functional theory calculations with in situ X‐ray diffraction reveal that combining Sb sites and oxygen vacancies prominently lessen the dimerization energy of adsorbed CO intermediate,thus boosting the conversion of CO_(2) to produce C_(2)H_(4).This study provides a new perspective for promoting selective C-C coupling for electrochemical CO_(2) reduction. | Senlin Chu Changwoo Kang Woonghyeon Park Yu Han Song Hong Leiduan Hao Hao Zhang Tsz Woon Benedict Lo Alex W.Robertson Yousung Jung Buxing Han Zhenyu Sun | 2022 | SmartMat2022，3，1： | 3 |
| 4 | 单原子配位结构及与载体相互作用的调控用于二氧化碳电催化还原显示文摘电催化二氧化碳还原(ECR)制备高值化学品被认为是在碳中和背景下实现可再生能源存储及降低CO浓度的一种有效策略。为了实现此目标,催化剂的开发与设计是ECR研究的关键。单原子催化剂(SACs)因其独特的电子结构、明确的配位环境和极高的原子利用率,近年来在ECR领域引起了广泛关注。通过调节SACs的中心金属元素种类和局部配位结构,可有效调节SACs对CO和其还原中间体的吸附强度和催化活性。本文总结了SACs在ECR领域所取得的最新研究进展,重点讨论了SACs的配位结构及其与载体之间的相互作用对催化活性的影响以及相关调控策略,最后,提出了SACs应用于ECR所面临的机遇与挑战。 | 陈宇新 王丽君 姚志波 郝磊端 谭心怡 Justus Masa Alex W.Robertson 孙振宇 | 2022 | 物理化学学报2022，38，11： | 2 |
| 5 | Prediction of Indian summer monsoon rainfall (ISMR) using canonical correlation analysis of global circulation model products显示文摘 | AnkitaSingh Makarand A.Kulkarni U. C.Mohanty S. C.Kar Andrew W.Robertson G.Mishra | 2012 | Met Apps2012，，2： | 1 |
| 6 | Engineering vacancy and hydrophobicity of two-dimensional TaTe_(2)for efficient and stable electrocatalytic N_(2)reduction显示文摘Demand for ammonia continues to increase to sustain the growing global population.The direct electrochemical N2 reduction reaction(NRR)powered by renewable electricity offers a promising carbon-neutral and sustainable strategy for manufacturing NH3,yet achieving this remains a grand challenge.Here,we report a synergistic strategy to promote ambient NRR for ammonia production by tuning the Te vacancies(VTe)and surface hydrophobicity of two-dimensional TaTe_(2)nanosheets.Remarkable NH3 faradic efficiency of up to 32.2%is attained at a mild overpotential,which is largely maintained even after 100 h of consecutive electrolysis.Isotopic labeling validates that the N atoms of formed NH4+originate from N2.In situ X-ray diffraction indicates preservation of the crystalline structure of TaTe_(2)during NRR.Further density functional theory calculations reveal that the potential-determining step(PDS)is*NH_(2)+(H^(+)+e^(-))/NH3 on VTe-TaTe_(2)compared with that of*+N2+(H^(+)+e^(-))/*N-NH on TaTe_(2).We identify that the edge plane of TaTe_(2)and VTe serve as the main active sites for NRR.The free energy change at PDS on VTe-TaTe_(2)is comparable with the values at the top of the NRR volcano plots on various transition metal surfaces. | Zhenqing Zhao Jongseo Park Changhyeok Choi Song Hong Xiangchao Hui Hao Zhang Tsz Woon Benedict Lo Alex W.Robertson Zengxiang Lv Yousung Jung Zhenyu Sun | 2022 | The Innovation2022，3，1： | 1 |
| 7 | Ru单原子电催化固氮显示文摘文章简介在温和条件下实现固氮仍然是一个巨大的挑战。本工作报道了室温常压下钌(Ru)单原子电催化固氮,担载于氮掺杂多孔碳上的Ru单分散位点极大地促进了水溶液中N2的电化学还原,选择性地生成NH3,在-0.21 V(相对于可逆氢电极,RHE)电位下获得3.665 mgNH3h-1 mg-1Ru的NH3产率。 | 陶亨聪 Changhyeok Choi Liang-Xin Ding Zheng Jiang Zishan Han Mingwen Jia Qun Fan Yunnan Gao 王海辉 Alex W.Robertson Song Hong Yousung Jung Shizhen Liu 孙振宇 | 2020 | 科学新闻2020，，2： | 0 |
| 8 | Ultrafine MoO_(x)clusters anchored on g-C_(3)N_(4)with nitrogen/oxygen dual defects for synergistic efficient O_(2)activation and tetracycline photodegradation显示文摘Photocatalytic O_(2)activation to generate reactive oxygen species is crucially important for purifying organic pollutants,yet remains a challenge due to poor adsorption of O_(2)and low efficiency of electron transfer.Herein,we demonstrate that ultrafine MoO_(x)clusters anchored on graphitic carbon nitride(g-C_(3)N_(4))with dual nitrogen/oxygen defects promote the photocatalytic activation of O_(2)to generate·O_(2)−for the degradation of tetracycline hydrochloride(TCH).A range of characterization techniques and density functional theory(DFT)calculations reveal that the introduction of the nitrogen/oxygen dual defects and MoO_(x)clusters enhances the O_(2)adsorption energy from−2.77 to−2.94 eV.We find that MoO_(x)clusters with oxygen vacancies(Ov)and surface Ov-mediated Moδ+(3≥δ≥2)possess unpaired localized electrons,which act as electron capture centers to transfer electrons to the MoO_(x)clusters.These electrons can then transfer to the surface adsorbed O_(2),thus promoting the photocatalytic conversion of O_(2)to·O_(2)−and,simultaneously,realizing the efficient separation of photogenerated electron–hole pairs.Our fully-optimized MoO_(x)/g-C_(3)N_(4)catalyst with dual nitrogen/oxygen defects manifests outstanding photoactivities,achieving 79%degradation efficiency toward TCH within 120 min under visible light irradiation,representing nearly 7 times higher activity than pristine g-C_(3)N_(4).Finally,based on the results of liquid chromatograph mass spectrometry and DFT calculations,the possible photocatalytic degradation pathways of TCH were proposed. | Huidong Shen Xinyu Zhan Song Hong Liang Xu Chunming Yang Alex W.Robertson Leiduan Hao Feng Fu Zhenyu Sun | 2023 | Nano Research2023，16，8： | 0 |
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