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Progress in tracking electrochemical CO2 reduction intermediates over single-atom catalysts using operando ATR-SEIRAS 利用操作式 ATR-SEIRAS 追踪单原子催化剂上的二氧化碳电化学还原中间产物的研究进展
IF 15.7 1区 化学 Q1 CHEMISTRY, APPLIED Pub Date : 2024-07-01 DOI: 10.1016/S1872-2067(24)60068-9

Owing to the multiple proton-coupled electron transfer steps involved in the electrochemical carbon dioxide reduction reaction (CO2RR), single-atom catalysts (SACs) are ideal platforms for studying such complex chemical reaction processes. The structural simplicity and homogeneity of SACs facilitate the understanding of the structure-performance relationship and reaction mechanisms of the CO2RR. Operando attenuated total reflection surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) is a valuable tool to identify the dynamic intermediate transformation processes in the CO2RR occurring on SACs and to study the impact of local reaction environments on the CO2RR performance. This article reviews operando ATR-SEIRAS and its key applications in the SAC-catalyzed CO2RR. The review briefly introduces the surface enhancement mechanism of electrochemical in situ infrared spectroscopy, formation mechanisms of the C1 and C2 products, function of operando ATR-SEIRAS in investigating the mechanisms of single-/dual-atom catalysts in converting CO2/CO to C1 and C2 products, and methods of using spectroscopic information to determine the interfacial H2O and local pH at the electrode. Finally, the review provides perspectives on the future development of operando ATR-SEIRAS.

由于电化学二氧化碳还原反应(CO2RR)涉及多个质子耦合电子转移步骤,单原子催化剂(SAC)是研究此类复杂化学反应过程的理想平台。单原子催化剂(SAC)的结构简单、均匀,有助于了解二氧化碳还原反应的结构-性能关系和反应机理。操作型衰减全反射表面增强红外吸收光谱(ATR-SEIRAS)是一种宝贵的工具,可用于识别发生在 SACs 上的 CO2RR 动态中间转化过程,并研究局部反应环境对 CO2RR 性能的影响。本文回顾了操作型 ATR-SEIRAS 及其在 SAC 催化 CO2RR 中的主要应用。综述简要介绍了电化学原位红外光谱的表面增强机制、C1 和 C2 产物的形成机制、操作式 ATR-SEIRAS 在研究单/双原子催化剂将 CO2/CO 转化为 C1 和 C2 产物的机制中的作用,以及利用光谱信息确定电极界面 H2O 和局部 pH 值的方法。最后,综述对操作型 ATR-SEIRAS 的未来发展进行了展望。
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引用次数: 0
Surface dynamics of Rh/Al2O3 during propane dehydrogenation 丙烷脱氢过程中 Rh/Al2O3 的表面动力学
IF 15.7 1区 化学 Q1 CHEMISTRY, APPLIED Pub Date : 2024-07-01 DOI: 10.1016/S1872-2067(24)60063-X

The surface structures of heterogeneous catalysts significantly impact catalytic performance, especially for structure-sensitive reactions. In this study, we employed surface techniques such as low-energy ion scattering spectroscopy, X-ray photoelectron spectroscopy, and Fourier transform infrared spectroscopy with CO as a probe (CO-FTIR) to investigate the surface dynamics of Rh/Al2O3 catalysts for propane dehydrogenation (PDH). We observed a notable induction process for PDH on Rh/Al2O3 catalysts, marked by significant variations in propane conversion, methane, and propylene selectivities. These changes were attributed to substantial coke formation. Aberration-corrected high-angle annular dark-field scanning transmission electron microscopy) and CO-FTIR revealed the coexistence of Rh nanoparticles, clusters, and single atoms on the surface. Through various dynamic quasi in-situ characterizations, we found that coke preferentially covered Rh clusters, thereby inhibiting C–C bond breaking and methane formation. Meanwhile, Rh single atoms were less affected by coke coverage and remained exposed as active and selective sites for PDH, favoring propylene production. This work underscores the sensitivity of PDH to the sizes of Rh species, with isolated Rh single atoms promoting propylene formation.

异相催化剂的表面结构对催化性能有很大影响,尤其是对结构敏感的反应。在本研究中,我们采用了低能离子散射光谱、X 射线光电子能谱和以 CO 为探针的傅立叶变换红外光谱(CO-FTIR)等表面技术来研究用于丙烷脱氢(PDH)的 Rh/Al2O3 催化剂的表面动力学。我们在 Rh/Al2O3 催化剂上观察到了明显的 PDH 诱导过程,其特点是丙烷转化率、甲烷和丙烯选择性的显著变化。这些变化归因于大量焦炭的形成。畸变校正高角度环形暗场扫描透射电子显微镜)和 CO-FTIR 揭示了表面上 Rh 纳米颗粒、团簇和单原子的共存。通过各种动态准原位表征,我们发现焦炭优先覆盖了 Rh 簇,从而抑制了 C-C 键的断裂和甲烷的形成。同时,Rh 单原子受焦炭覆盖的影响较小,仍作为 PDH 的活性和选择性位点暴露在外,有利于丙烯的生成。这项研究强调了 PDH 对 Rh 物种大小的敏感性,孤立的 Rh 单原子可促进丙烯的形成。
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引用次数: 0
Manipulating the interactions between N-intermediates and one-dimensional conjugated coordination polymers to boost electroreduction of nitrate to ammonia 操纵 N-中间体与一维共轭配位聚合物之间的相互作用,促进硝酸盐到氨的电还原反应
IF 15.7 1区 化学 Q1 CHEMISTRY, APPLIED Pub Date : 2024-07-01 DOI: 10.1016/S1872-2067(24)60059-8

Electrocatalytic reduction of nitrate to ammonia (NITRR) is a promising strategy to remove nitrate pollutants and generate ammonia under mild conditions. However, the low conversion rate of nitrate and insufficient ammonia production rate severely limits the development of NITRR. Manipulating the adsorption of N-intermediates on the surface of catalyst greatly affects the activity and the selectivity of catalytic reaction. Herein, four one-dimensional π-d conjugated coordination polymers (1D CCPs) are synthesized and applied to NITRR. The selectivity and activity of NITRR are well improved by metal ion substitutions, which regulate the adsorption towards generated intermediates. The ammonia production rate reaches 2.28 mg h–1 cm–2 over Cu-BTA in 2 h, comparable to recent works at low nitrate concentrations, and the conversion rate of nitrate up to 96.74% in four hours with 79.46% ammonia selectivity. Density functional theory calculations reveal that Cu-BTA had electron-richer Cu center, causing the enhanced free energy of *NO and the attenuation of N=O bond. Therefore, the ΔG required for converting *NO to *NHO is reduced and the further hydrogenation is promoted. Additionally, the adsorption energies toward NH3 are also effectively reduced by metal ions substitution, accelerating the desorption of generated and adsorbed NH3, making the turnover of catalysts more frequent.

电催化硝酸盐还原成氨(NITRR)是一种在温和条件下去除硝酸盐污染物并生成氨的可行策略。然而,硝酸盐转化率低和氨生成率不足严重限制了 NITRR 的发展。操纵催化剂表面对 N 介质的吸附会极大地影响催化反应的活性和选择性。本文合成了四种一维π-d共轭配位聚合物(1D CCPs),并将其应用于 NITRR。通过金属离子的置换,NITRR 的选择性和活性得到了很好的改善。Cu-BTA 在 2 小时内的氨生产率达到 2.28 毫克/小时-1 厘米-2,与最近在低浓度硝酸盐条件下的研究结果相当;硝酸盐在 4 小时内的转化率高达 96.74%,氨选择性为 79.46%。密度泛函理论计算显示,Cu-BTA 具有更强电子的 Cu 中心,导致 *NO 自由能增强,N=O 键衰减。因此,将 *NO 转化为 *NHO 所需的ΔG 降低了,从而促进了进一步的氢化。此外,金属离子的取代也有效降低了对 NH3 的吸附能,加速了生成和吸附的 NH3 的解吸,使催化剂的周转更加频繁。
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引用次数: 0
Recent advances of the catalysts for photoelectrocatalytic oxygen evolution and CO2 reduction reactions 光电催化氧进化和二氧化碳还原反应催化剂的最新进展
IF 15.7 1区 化学 Q1 CHEMISTRY, APPLIED Pub Date : 2024-07-01 DOI: 10.1016/S1872-2067(24)60053-7

Increasing global energy consumption and environmental pollution make the use of new energy sources and environmentally friendly technologies essential to meet the diverse needs of industries. Photoelectrocatalysis is a promising method of utilising solar and electrical energy for various catalytic reactions with significant environmental and energy saving benefits. And photoelectrocatalytic (PEC) oxygen evolution reaction (OER) and CO2 reduction reaction (CO2RR) are two catalytic reactions with great potential for energy and environmental applications. PEC OER is critical for renewable energy technologies for water oxidation and other related oxidation reactions. PEC CO2RR converts carbon dioxide into high-value products via a catalyst, enabling the rational use of carbon dioxide and the reduction of greenhouse gas emissions. Both technologies are efficient, environmentally friendly, and sustainable. However, further research and optimisation are needed to promote the industrial application of both technologies for energy conversion and environmental protection. This paper reviews the research progress of PEC CO2RR and OER catalysts in recent years, including detailed descriptions of catalyst types, reaction mechanisms and performance tests. Finally, the paper considers the future trends and prospects of PEC technology, providing new insights into the technology and research directions for PEC OER and CO2RR catalysts.

全球能源消耗和环境污染日益严重,因此必须利用新能源和环保技术来满足各行各业的不同需求。光电催化是一种利用太阳能和电能进行各种催化反应的可行方法,具有显著的环保和节能优势。光电催化(PEC)氧进化反应(OER)和二氧化碳还原反应(CO2RR)是两种在能源和环境应用方面具有巨大潜力的催化反应。PEC 氧进化反应对于可再生能源技术中的水氧化和其他相关氧化反应至关重要。PEC CO2RR 通过催化剂将二氧化碳转化为高价值产品,从而实现二氧化碳的合理利用,减少温室气体排放。这两种技术都具有高效、环保和可持续的特点。然而,要促进这两种技术在能源转换和环境保护方面的工业应用,还需要进一步的研究和优化。本文回顾了近年来 PEC CO2RR 和 OER 催化剂的研究进展,包括催化剂类型、反应机理和性能测试的详细介绍。最后,本文探讨了 PEC 技术的未来发展趋势和前景,为 PEC OER 和 CO2RR 催化剂的技术和研究方向提供了新的见解。
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引用次数: 0
Coordination dynamics of iron enables the selective C–N coupling but bypasses unwanted C–H hydroxylation in Fe(II)/α-ketoglutarate- dependent non-heme enzymes 铁的配位动力学使铁(II)/α-酮戊二酸依赖性非血红素酶中的选择性 C-N 偶联得以实现,但绕过了不需要的 C-H 羟基化反应
IF 15.7 1区 化学 Q1 CHEMISTRY, APPLIED Pub Date : 2024-07-01 DOI: 10.1016/S1872-2067(24)60064-1

Non-heme Fe(II)/α-ketoglutarate (αKG)-dependent enzymes catalyze numerous C–H activation and functionalization reactions. However, how αKG-dependent non-heme enzymes catalyzed C–H functionalization beyond the hydroxylation is largely unknown. Here, we addressed this issue in Fe(II)/ αKG-dependent oxygenase TqaLNc, which catalyzes the selective C–H amination but bypasses the thermodynamically favored C–H hydroxylation. Here, the extensive computational studies have shown that the aziridine formation involves the conformational change of the Fe(IV)=O species from the axial configuration to the equatorial one, the substrate deprotonation of NH3+ group to form the NH-ligated intermediate, the C–H activation by the equatorial Fe(IV)=O species. Such mechanistic scenario has been cross-validated by oxidation of various substrates by TqaLNc and its variants, including the available experiments and our new experiments. While the presence of steric hindrance between the substrate and the second-sphere residues would inhibit the aziridination process, the intrinsic reactivity of aziridination vs. hydroxylation is dictated by the energy splitting between two key redox-active dπ* frontier molecular orbitals: dπ*Fe-N and dπ*Fe-OH. The present findings highlight the key roles of the coordination change and dynamics of iron cofactor in dictating the catalysis of non-heme enzymes and have far-reaching implications for the other non-heme Fe(II)/αKG-dependent enzymes catalyzed C–H functionalization beyond the hydroxylation.

非血红素 Fe(II)/α-Ketoglutarate (αKG) 依赖性酶催化了许多 C-H 活化和官能化反应。然而,除了羟基化反应之外,依赖 αKG 的非血红素酶如何催化 C-H 功能化在很大程度上还是未知数。在这里,我们在依赖铁(II)/αKG 的加氧酶 TqaLNc 中解决了这一问题,该酶催化选择性 C-H 氨基化,但绕过了热力学上有利的 C-H 羟基化。大量的计算研究表明,氮丙啶的形成涉及到 Fe(IV)=O 物种从轴向构型到赤道构型的构象变化、底物 NH3+ 基团的去质子化形成 NH-配位中间体、赤道 Fe(IV)=O 物种的 C-H 活化。通过 TqaLNc 及其变体氧化各种底物,包括现有实验和我们的新实验,这种机理设想得到了交叉验证。虽然底物与第二球残基之间存在的立体阻碍会抑制叠氮化过程,但叠氮化与羟基化的内在反应性是由两个关键的氧化还原活性 dπ* 前沿分子轨道(dπ*Fe-N 和 dπ*Fe-OH)之间的能量分裂决定的。本研究结果突显了铁辅助因子的配位变化和动力学在非血红素酶催化过程中的关键作用,并对其他非血红素 Fe(II)/αKG 依赖性酶催化羟基以外的 C-H 功能化具有深远影响。
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引用次数: 0
Proton feeding from defect-rich carbon support to cobalt phthalocyanine for efficient CO2 electroreduction 从富含缺陷的碳支持物向酞菁钴提供质子,实现高效的二氧化碳电还原
IF 15.7 1区 化学 Q1 CHEMISTRY, APPLIED Pub Date : 2024-07-01 DOI: 10.1016/S1872-2067(24)60061-6

Electrocatalytic CO2 reduction reaction (CO2RR) holds significant promise for sustainable energy conversion, with cobalt phthalocyanine (CoPc) emerging as a notable catalyst due to its high CO selectivity. However, CoPc's efficacy is hindered by its limited ability to provide sufficient proton for the protonation process, particularly at industrial current densities. Herein, we introduce defect-engineered carbon nanotubes (d-CNT) to augment proton feeding for CO2RR over CoPc, achieved by expediting water dissociation. Our kinetic measurements and in-situ attenuated total reflection surface-enhanced infrared absorption spectroscopy reveal d-CNT significantly enhances proton feeding, thereby facilitating CO2 activation to *COOH in CoPc. Density functional theory calculations corroborate these findings, illustrating that d-CNT decreases the barrier to water dissociation. Consequently, the CoPc/d-CNT mixture demonstrates robust performance, achieving 500 mA cm–2 for CO2RR with CO selectivity exceeding 96%. Notably, CoPc/d-CNT remains stability for a duration of 20 h under a substantial current density of 150 mA cm–2. The study broadens the scope of practical applications for molecular catalysts in CO2RR, marking a significant step towards sustainable energy conversion.

电催化二氧化碳还原反应(CO2RR)在可持续能源转换方面大有可为,其中酞菁钴(CoPc)因其高二氧化碳选择性而成为一种引人注目的催化剂。然而,CoPc 为质子化过程提供足够质子的能力有限,这阻碍了它的功效,尤其是在工业电流密度下。在此,我们引入了缺陷工程碳纳米管(d-CNT),通过加速水的解离来增加 CO2RR 对 CoPc 的质子供给。我们的动力学测量和原位衰减全反射表面增强红外吸收光谱显示,d-CNT 能显著增强质子馈入,从而促进 CO2 在 CoPc 中活化为 *COOH。密度泛函理论计算证实了这些发现,说明 d-CNT 降低了水解离的障碍。因此,CoPc/d-CNT 混合物表现出强劲的性能,CO2RR 达到 500 mA cm-2,CO 选择性超过 96%。值得注意的是,在 150 mA cm-2 的大电流密度下,CoPc/d-CNT 可在 20 小时内保持稳定。这项研究拓宽了分子催化剂在 CO2RR 中的实际应用范围,标志着向可持续能源转换迈出了重要一步。
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引用次数: 0
Rational design of Pt-anchored single-atom alloy electrocatalysts for NO-to-NH3 conversion by density functional theory and machine learning 通过密度泛函理论和机器学习合理设计用于 NO-NH3 转化的铂锚定单原子合金电催化剂
IF 15.7 1区 化学 Q1 CHEMISTRY, APPLIED Pub Date : 2024-07-01 DOI: 10.1016/S1872-2067(24)60078-1

Electrochemical NO reduction reaction (NORR) toward NH3 synthesis emerges as a promising approach to eliminate NO pollution and generate high-value-added products simultaneously. Therefore, exploring suitable NORR electrocatalysts is of great importance. Here, we present a design principle to evaluate the activity of single-atom alloy catalysts (SAACs), whose excellent catalytic performance and well-defined bonding environments make them suitable candidates for studying structure-activity relationships. The machine learning (ML) algorithm is chosen to unveil the underlying physics and chemistry. The results indicate that the catalytic activity of SAACs is highly correlated with the local environment of the active center, that is, the atomic and electronic features. The coeffect of these features is quantitatively verified by adopting a data-driven method. The combination of density functional theory (DFT) and ML investigations not only provides an understanding of the complex NORR mechanisms but also offers a strategy to design highly efficient SAACs with specific active centers rationally.

为合成 NH3 而进行的电化学 NO 还原反应(NORR)是消除 NO 污染并同时生成高附加值产品的一种前景广阔的方法。因此,探索合适的 NORR 电催化剂非常重要。单原子合金催化剂(SAACs)具有优异的催化性能和明确的键合环境,是研究结构-活性关系的合适候选材料,在此,我们提出了一种评估单原子合金催化剂(SAACs)活性的设计原理。研究选择了机器学习(ML)算法来揭示其背后的物理和化学原理。结果表明,SAACs 的催化活性与活性中心的局部环境,即原子和电子特征高度相关。采用数据驱动方法定量验证了这些特征的协同效应。密度泛函理论(DFT)与 ML 研究的结合不仅有助于理解复杂的 NORR 机理,还为合理设计具有特定活性中心的高效 SAAC 提供了一种策略。
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引用次数: 0
Large-current polarization-engineered FeOOH@NiOOH electrocatalyst with stable Fe sites for large-current oxygen evolution reaction 具有稳定铁位点的大电流极化工程化 FeOOH@NiOOH 电催化剂用于大电流氧进化反应
IF 15.7 1区 化学 Q1 CHEMISTRY, APPLIED Pub Date : 2024-07-01 DOI: 10.1016/S1872-2067(24)60062-8

NiFe-based (oxy)hydroxides are among the most efficient electrocatalysts for the oxygen evolution reaction (OER). However, significant Fe leakage during the OER results in unsatisfactory stability. Herein, a large-current (1.5 A cm–2) galvanostatic reconstruction was used to fabricate FeOOH@NiOOH (eFNOL) with both fixed Fe sites and exposed high-index crystal facets (HIFs). Compared to FeNiOOH with low-index crystal facets, the phase-separated FeOOH@NiOOH showed a higher binding energy towards Fe, and the HIFs significantly improved the catalytic activity of FeOOH. The optimized eFNOL catalyst exhibits ultralow overpotentials of 234 and 272 mV, yielding substantial current densities of 100 and 500 mA cm–2, respectively, with a small Tafel slope of 35.2 mV dec–1. Moreover, due to the stabilized Fe sites, its striking stability over 100 h at 500 mA cm–2 with 1.5% decay outperforms most NiFe-based OER catalysts reported recently. This study provides an effective strategy for developing highly active and stable catalysts via large-current electrochemical reconstruction.

镍铁基(氧)氢氧化物是氧进化反应(OER)中最高效的电催化剂之一。然而,OER 过程中铁的大量泄漏导致其稳定性不尽人意。本文采用大电流(1.5 A cm-2)电静电重构法制备了具有固定铁位点和外露高指数晶面(HIF)的 FeOOH@NiOOH(eFNOL)。与低指数晶面的 FeNiOOH 相比,相分离的 FeOOH@NiOOH 显示出更高的铁结合能,HIF 显著提高了 FeOOH 的催化活性。优化后的 eFNOL 催化剂显示出 234 和 272 mV 的超低过电位,产生的可观电流密度分别为 100 和 500 mA cm-2,塔菲尔斜率较小,为 35.2 mV dec-1。此外,由于铁位点的稳定,该催化剂在 500 mA cm-2 电流下 100 小时内的稳定性惊人,衰减率仅为 1.5%,优于最近报道的大多数镍铁基 OER 催化剂。这项研究为通过大电流电化学重构开发高活性、高稳定性催化剂提供了一种有效的策略。
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引用次数: 0
An efficient and stable high-entropy alloy electrocatalyst for hydrogen evolution reaction 用于氢气进化反应的高效稳定的高熵合金电催化剂
IF 15.7 1区 化学 Q1 CHEMISTRY, APPLIED Pub Date : 2024-07-01 DOI: 10.1016/S1872-2067(24)60067-7

High-entropy alloy (HEA) catalysts exhibit enhanced hydrogen evolution reaction (HER) activity in water electrolysis, yet the understanding of their structure and active sites in reaction environments remains unclear. Here, we systematically investigated the HER activity and stability of PtPdRhRuCu/C through a combination of electrochemical measurements, in situ synchrotron radiation X-ray absorption spectroscopy (XAS) at the Cu K-edge and Pt L3-edge, and density functional theory (DFT) calculations. Uniformly sized PtPdRhRuCu HEA nanoparticles were prepared via a facile one-step solvothermal method. In situ XAS results revealed that the HEA nanoparticles maintained metallic states and a disordered arrangement of the overall structure at hydrogen evolution potential, implying the absence of the separated phases. Relying on multi-metal active sites, PtPdRhRuCu/C demonstrated a remarkably low overpotential of 23.3 mV at 10 mA cm–2 in alkaline HER, which is significantly lower than the overpotential observed in commercial Pt/C (50.3 mV), and achieving a mass activity 7.9 times that of Pt/C. DFT calculations show that the synergy of each metal site optimizes the dissociation energy barrier of water molecules. This study not only demonstrates the advancement of high-entropy alloys in electrocatalysis but also provides a comprehensive understanding of the structure-activity relationship of these unique catalysts through detailed characterizations. Our findings further contribute to the rational design and application of high-entropy alloy catalysts, specifically in HER.

高熵合金(HEA)催化剂在电解水过程中表现出更强的氢进化反应(HER)活性,但人们对其结构和反应环境中的活性位点的了解仍不清楚。在此,我们结合电化学测量、铜 K 边和铂 L3 边的原位同步辐射 X 射线吸收光谱 (XAS) 以及密度泛函理论 (DFT) 计算,系统地研究了 PtPdRhRuCu/C 的氢进化反应活性和稳定性。通过简单的一步溶热法制备了大小均匀的 PtPdRhRuCu HEA 纳米粒子。原位 XAS 结果表明,在氢进化电位下,HEA 纳米粒子保持金属态,整体结构排列无序,这意味着不存在分离相。依靠多金属活性位点,PtPdRhRuCu/C 在碱性 HER 中的过电位非常低,在 10 mA cm-2 的条件下仅为 23.3 mV,大大低于在商用 Pt/C 中观察到的过电位(50.3 mV),其质量活性是 Pt/C 的 7.9 倍。DFT 计算表明,每个金属位点的协同作用优化了水分子的解离能垒。这项研究不仅证明了高熵合金在电催化领域的先进性,还通过详细的表征全面了解了这些独特催化剂的结构-活性关系。我们的发现进一步促进了高熵合金催化剂的合理设计和应用,特别是在 HER 中的应用。
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引用次数: 0
Synergistic photoelectric and thermal effect for efficient nitrate reduction on plasmonic Cu photocathodes 等离子铜光电阴极上高效硝酸盐还原的光电和热协同效应
IF 15.7 1区 化学 Q1 CHEMISTRY, APPLIED Pub Date : 2024-07-01 DOI: 10.1016/S1872-2067(24)60060-4

Recently, electrochemical nitrate reduction reaction (NO3RR) has been intensively explored for the synthesis of ammonia, and copper (Cu) has become one of the most promising materials for NO3RR. Notably, Cu is an important plasmonic metal that absorbs visible light. The plasmonic effect might have a significant influence on the performance of Cu-catalyzed NO3RR but has been seldom reported. Herein, we report the synergistic photoelectric and thermal effect for efficient and stable NO3RR on plasmonic Cu nanowire photocathodes, which is exclusively effective for NO3RR but has no effect on the competing hydrogen evolution reaction. The faradaic efficiency for ammonia production is nearly 100% within a potential range from –0.2 V to –0.4 V vs. RHE, and a high ammonia yield rate of 1.37 mmol h–1 cm–2 is achieved at –0.2 V vs. RHE. Further operando photoelectrochemical studies and theoretical simulations confirm that the plasmonic excitation efficiently accelerates the rate-limiting desorption of NH3 on Cu surfaces. We further demonstrate the versatility of this strategy to other Cu-based nanostructures.

最近,人们对电化学硝酸盐还原反应(NO3RR)合成氨进行了深入探讨,而铜(Cu)已成为最有前途的 NO3RR 材料之一。值得注意的是,铜是一种能吸收可见光的重要等离子金属。质子效应可能会对铜催化 NO3RR 的性能产生重大影响,但却鲜有报道。在此,我们报告了在等离子体铜纳米线光电阴极上高效稳定的 NO3RR 的光电和热协同效应,该效应只对 NO3RR 有效,但对竞争性的氢进化反应没有影响。在 -0.2 V 至 -0.4 V 的电位范围内,氨生产的法拉第效率接近 100%,而在 -0.2 V 的电位范围内,氨的产率高达 1.37 mmol h-1 cm-2。进一步的操作性光电化学研究和理论模拟证实,质子激发有效地加速了 NH3 在铜表面的限速解吸。我们进一步证明了这一策略在其他铜基纳米结构上的通用性。
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引用次数: 0
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Chinese Journal of Catalysis
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