Efficient Charge Separation Research Articles

TiN/TiO2 embedded in ReS2 nanoflowers with wide light absorption and multi-interfacial charge transfer for efficient photocatalytic hydrogen generation

The design of functional materials with efficient light absorption and charge separation is crucial for photocatalytic energy conversion. Herein, a plasmonic TiN/TiO2/ReS2 ternary hybrid is prepared, which exhibits exceptional photocatalytic activity caused by the plasmon-mediated light absorption and multi-interfacial charge separation. The ternary hybrids were synthesized by heating TiN, Re, and S sources at high pressure and temperature. The TiN was partially oxidized to form TiN/TiO2 hybrids, which were then embedded in ReS2 nanoflowers through Ti-S bonds, creating a 3D flower-like structure with multiple interfaces. The plasmon resonance of TiN and the bandgap excitations of ReS2 and TiO2 endow the hybrids with efficient light absorption in UV–VIS-NIR region. Additionally, the novel embedded structure and the multiple interfaces between TiN, TiO2, and ReS2 facilitate the formation of built-in electric fields and multi-channel charge transfer, which efficiently quicken photoinduced carriers’ migration and hot electron injection. Consequently, the TiN/TiO2/ReS2 hybrids demonstrate a high-efficiency photocatalytic hydrogen generation rate, which is 12.1 times that of commercial P25. Notably, the hybrids also exhibit high photocatalytic activity under near-infrared light irradiation. This study offers innovative insights into the design of photocatalysts and suggests that the prepared materials could be utilized in solar-driven energy conversion applications.

Re3P4@C/TiO2 Ohmic junction Boosts charge carrier separation for photocatalytic hydrogen evolution

Construction of heterostructures featuring a well-designed transport pathway is pivotal in regulating the behavior of charge carriers, thereby achieving boosted separation efficiency. One of the primary factors leading to poor charge transfer and separation efficiency in heterostructures lies in the presence of interface barriers that hinder their transfer. Establishing an Ohmic contact with a low energy barrier can significantly reduce charge transfer resistance during photocatalysis. In this contribution, we have successfully developed an Re3P4@C/TiO2 Ohmic junction for highly improved photocatalytic H2 evolution rate, which exhibited a 68-fold increase compared to pristine TiO2. Experimental results combined with density functional theory calculations confirm the successful construction of Ohmic junction, which effectively facilitates the separation and transfer of photogenerated charge carriers while prolongs their lifetimes. This heterojunction also enhances the adsorption capacity for reactants and thus promotes the surface photocatalytic reactions. This work provides valuable insights into novel Ohmic junction construction to improve the photocatalytic activity.

Self-Sensitization-Induced Protonation Sites for Weak-Light-Driven Hydrogen Evolution in Coordination Polymers

The exploration on weak-light-driven catalysis is an important approach to reduce the dependence of photocatalysts on strong light and improve the efficiency of solar spectrum utilization. However, the reported photocatalysts typically necessitate high light intensity (e.g., exceeding 100mWcm−2) for catalytic reactions, which cannot be achieved with natural solar light. Herein, a self-sensitization-induced strategy was employed to generate in-situ proton sites, enabling photocatalytic hydrogen evolution reaction (HER) even under low light intensity (10mWcm−2). An indolocarbazole ligand (H2ICDB) was utilized to construct a paddle-wheel dicopper coordination polymer (CuICDB-DMF). By substituting the axially coordinated DMF with methanol or water, CuICDB-MeOH and CuICDB-H2O were obtained. Under weak-light irradiation (10mWcm−2), CuICDB-H2O exhibited the highest photocatalytic HER rate of 838.4 μmol g−1 h−1 when compared to the other two counterparts. Remarkably, the substitution of axially coordinated H2O promotes charge separation and transfer efficiency through optimizing ligand-to-cluster charge transfer (LCCT) process. Moreover, density functional theory (DFT) calculations reveal that coordinated H2O substitution decreases the Gibbs free energy difference of the potential determining step (H2O* → OH* + H*) in CuICDB-H2O.

Enhanced charge transfer through defect and doping synergistic engineering for efficient hydrogen production

Simultaneous modification of catalysts by surface defects and atomic doping strategies can effectively inhibit the recombination of photogenerated carriers. In this study, the surface state of MoS2 was adjusted through the synergistic effects of sulfur defects and the doping of oxygen atoms, successfully constructing a type II heterojunction with hydrogen-substituted graphdiyne (H-GDY) for efficient photocatalytic hydrogen generation. The results showed that the H-GDY/O-MoS2-x exhibits the best hydrogen production performance (2272.97 μmol/g/h), which is about 25 times that of MoS2. And the synergistic effect of sulfur defects and oxygen doping engineering can modulate the energy band structure and increase the interfacial potential difference between H-GDY and O-MoS2-x, which enhances the driving force of electron transfer and improves the interfacial charge transfer and separation efficiency. This work shows that the synergistic effect of defect and doping engineering can effectively improve the photocatalytic performance and provides a new idea for the preparation of sulfide-based photocatalysts.

Fermi energy level synergistic Bi-based electron bridge construction of Z-type heterojunctions to accelerated photogenerated charge transfer for photostability and contaminant mineralization

Advanced oxidation technologies offer new opportunities for pollutant degradation. Despite the existence of numerous photocatalyst heterojunctions for advanced oxidation, their charge transfer and separation efficiency is low due to inadequate interfacial modulation, especially for Type II heterojunctions. Here, through metal reduction, metal defects with regulating the Fermi level and metal electron bridges with facilitate the separation of photo-generated carriers, facilitating the transition from Type II to Z-type heterojunctions. Herein, we designed a Z-Scheme photocatalyst with Bi-based electron bridges (referred to as ‘fishbone-like’ BiVO4/Bi/CuO) synthesized through in situ reduction, utilized for RhB degradation. Under visible light irradiation, the degradation rate of RhB up to 99 % within 120 min, outperforming most previously reported photocatalysts. Notably, the well-designed BiVO4/Bi/CuO exhibits as reaction rate of 4.13 × 10-2 ·min−1, which is 18 times higher than the pure BiVO4. The BiVO4/Bi/CuO photocatalyst demonstrates exceptional stability over 6 reaction cycles spanning 15 h, due to strengthened contact interface of BiVO4/Bi/CuO. The metal Bi can induce the surface plasmon resonance (SPR) effect, enhancing light absorption. Furthermore, Bi-based electron bridges significantly promote the charge transfer across the Z-type heterojunction interface, which were verified by assorted experimental outcomes and density functional theory (DFT) calculations. This work represents a promising platform for the development of highly efficient and stable photocatalysts that have potential in Pollutant degradation applications.

Hyaluronic acid modified prussian blue analogs/TiO₂ janus nanostructures through efficient charge separation to enhance photocatalytic-driven dual gas for achieve multimodal treatment of rheumatoid arthritis

Rheumatoid arthritis (RA) is a chronic autoimmune disease characterized by the abnormal proliferation of fibroblast-like synoviocytes and changes in the joint synovium, including elevated reactive oxygen species, decreased pH, and reduced oxygen content. In this study, we synthesized a novel nanocomposite material, namely HA-PBA-TiO2 Janus nanocomposite, by in situ etching in prussian blue analogs doped with Co and Ni, followed by the growth of TiO2 nano-flowers and encapsulation in hyaluronic acid. When these janus nanoparticles diffused to the inflammatory sites of RA, they exhibited outstanding photocatalytic water-splitting ability under 660 nm laser irradiation, generating H2 and O2. This capability helps ameliorate the hypoxic microenvironment at RA inflammatory sites by eliminating reactive oxygen species (ROS) and enhancing antioxidation and oxygenation. Furthermore, owing to the doping of Co and Ni, HA-PBA-TiO2 exhibits photothermal conversion capability, which significant damage to FLS upon exposure to 660 nm laser irradiation, thereby controlling their aberrant proliferation. Through a series of in vitro and in vivo experiments, we validated the significant therapeutic efficacy of HA-PBA-TiO2 in treating RA, highlighting its broad prospects for application.

Rational design of Z-scheme configured polymeric carbon nitride-decorated ZnWO4 nanofibers for enhanced visible-light-driven photodegradation of antibiotics

In this study, a Z-scheme heterostructure was meticulously engineered between zinc tungstate (ZnWO4) nanofibers and polymeric carbon nitride (PCN) nanosheets to augment the photocatalytic degradation of tetracycline (TC) under visible light irradiation. A cohesively integrated PCN/ZnWO4 photocatalyst structure was synthesized through an in-situ gas-solid reaction. The quantity and spatial distribution of PCN nanosheets were modulated by fine-tuning the gas precursor and reaction parameters. Relative to pristine ZnWO4 nanofibers and PCN photocatalysts, the distinct three-dimensional PCN/ZnWO4 heterostructure manifests a notable enhancement in photocatalytic performance, attributed to its plethora of active sites and a Z-scheme configuration that bolsters charge separation efficiency, achieving a tetracycline degradation rate of 95.4% upon exposure to simulated sunlight for 160 minutes. The employment of gas-solid reaction as a design paradigm pioneers a fresh paradigm in the strategic assembly of Z-scheme heterostructured photocatalysts, thereby illuminating a promising pathway for advancements in environmental remediation technologies.

Synthesis of CuOQDs/g-C3N4/C Composites Via Stem Template Induction and their Photocatalytic Properties

Introduction: The synthesis of bio-templated porous CuOQDs/g-C3N4/C composites with controllable morphology and suitable energy band structure was successfully carried out via a simple thermal condensation and hydrothermal method. Method: Dicyandiamide and cadmium chloride were selected as starting materials, while Hollyhock stem was chosen as the biological template. The results indicated that, in comparison to pure g-C3N4, g-C3N4/C had a rich porous structure and better-photogenerated carrier separation efficiency. The CuOQDs were anchored evenly on the surface of the g-C3N4, thus resulting in the formation of a greater number of reactive sites. Results: The type-Z heterojunction formed between the CuOQDs and g-C3N4/C reduced the energy required for electron transition, thereby facilitating the separation of photo-generated electronhole pairs. The highest photocatalytic degradation efficiency of CuOQDs/g-C3N4/C for tetracycline (TC) was 65.1%, which was 3.3 times that of pure g-C3N4. Conclusion: In the photocatalytic process, the main reactive species is O2−. The CuOQDs/g- C3N4/C synthesized by stem induction in multi-phase heterojunction form has a stable microstructure to improve the charge separation efficiency. Further, it represents practical photocatalytic environmental protection.

Boosted photocatalytic degradation performance of TiO2 with enriched oxygen vacancies

In this study, TiO2 with abundant oxygen vacancies (OVs) was prepared through a hydrothermal method in the presence of polyphenylsulphone (PPSU). Introduction of PPSU results in enriched OVs within TiO2 and boosted the level of ∙O2-, dramatically ameliorating photogenerated charges separation efficiency and elevating photocatalytic activity. Compared with the reference TiO2, PPSU-TiO2 exhibits enhance activity in photocatalytic degradation of rhodamine B (RhB) and tetracycline (TC). Analysis reveals that ∙O2- serves as the primary active free radicals in RhB degradation by PPSU-TiO2. Furthermore, PPSU-TiO2 maintains high activity over seven successive cycles, demonstrating excellent stability. Therefore, adding PPSU into the synthesis system of TiO2 is proved to be an effective strategy to enhance photocatalytic performance.

Anchoring AuCu alloy nanoparticles on TiO2 nanosheets: Exploiting synergistic effects and directed electron transfer for enhanced photocatalytic H2 evolution

AuCu/TiO2 composite photocatalysts were prepared by anchoring AuCu nanoparticles (NPs) on TiO2 nanosheets using a simple photoreduction method. Visible diffuse reflectance spectra indicated that the AuCu/TiO2 significantly enhanced light absorption in the visible region. Through photoluminescence spectroscopy and steady-state surface photovoltage experiments, AuCu/TiO2 exhibits an excellent photogenerated electron transfer rate. In addition, photoelectrochemical experiments showed that AuCu/TiO2 had a high photogenerated charge separation efficiency. AuCu/TiO2 (1.0 wt%) exhibited the best performance, under full spectrum, the hydrogen evolution rate is 33.94 mmol g−1 h−1, which is 1.59 times and 1.66 times higher than that of single metal Au/TiO2 (1.0 wt%) (21.28 mmol g−1 h−1) and Cu/TiO2 (1.0 wt%) (20.42 mmol g−1 h−1), respectively. The results showed that AuCu NPs greatly enhanced the photocatalytic performance of the composite photocatalysts.

Analyzing the Temperature Dependence of Titania Photocatalysis: Kinetic Competition between Water Oxidation Catalysis and Back Electron-Hole Recombination.

This study examines the kinetic origins of the temperature dependence of photoelectrochemical water oxidation on nanostructured titania photoanodes. We observe that the photocurrent is enhanced at 50 °C relative to 20 °C, with this enhancement being most pronounced (by up to 70%) at low anodic potentials (<+0.6 V vs RHE). Over this low potential range, the photocurrent magnitude is largely determined by kinetic competition between water oxidation catalysis (WOC) and recombination between surface holes and bulk electrons (back electron-hole recombination, BER). We quantify the BER process by transient photocurrent analyses under pulsed irradiation. Remarkably, we find that the kinetics of BER (∼90 ms half-time) are independent of temperature. In contrast, the kinetics of WOC, determined from the analysis of the photoinduced absorption of accumulated surface holes, are found to accelerate up to 2-fold at 50 °C relative to 20 °C. We conclude that the enhanced photocurrent densities observed in the low-applied potential region result primarily from the accelerated WOC, reducing losses due to the competing BER pathway. At higher applied potentials (>+0.6 V vs RHE), a smaller (∼10%) enhancement in photocurrent density is observed at 50 °C relative to 20 °C. Photoinduced absorption studies, correlated with studies using triethanolamine as a hole scavenger, indicate that this more modest enhancement at anodic potentials primarily results from an enhanced charge separation efficiency. We conclude by discussing the implications of these results for the practical application of photoanodic WOC under solar irradiation, influenced by these temperature-independent and -dependent underlying kinetic processes.

Bibliometric analysis of photocatalytic oxidation of volatile organic compounds from 1998 to 2023

IntroductionVolatile organic compounds (VOCs) have attracted widespread attention due to their adverse effects on human health. Photocatalytic oxidation is an effective technology for degrading VOCs under ambient conditions.MethodsIn order to better understand the trends and development of global trends in photocatalytic oxidation of VOCs, the analysis of 2493 articles or reviews from the Science Citation Index Expanded (SCIE) in the Web of Science Core Collection, covering the period from 1998 to 2023, was conducted using CiteSpace and VOSviewer software.Results and DiscussionThe findings indicate significant growth in papers concerning photocatalytic oxidation of VOCs. China emerges as the most active country among the main drivers. Principal sources publishing relevant research are Applied Catalysis B-Environmental, Chemical Engineering Journal, Journal of Hazardous Materials, and Environmental Science and Technology. A relatively well-established theoretical framework has been developed for the study of photocatalytic oxidation of VOCs. In the field of VOCs photocatalytic oxidation, the focus is on the development and optimization of advanced photocatalysts with efficient charge separation, better adsorption performance, and a wider light response range. In addition, the in-depth study of the charge generation and transfer mechanisms within the photocatalysts, as well as the comprehensive understanding of the reaction kinetics and catalytic oxidation process, the optimization of the reaction conditions, and the improvement of the catalytic efficiency are at the forefront of the research in this field. This research system is advancing and becoming more refined, with its theoretical propositions, research findings, and methodologies increasingly employed and confirmed.

Dual Electric Field Coupling with Tunable Schottky Barrier Synergistically Regulating Electronic Configuration in CoP@Ni‐CdS Heterojunction for Efficient Photocatalytic H2 Evolution

AbstractDesigning and exploiting visible‐light‐responsive materials that converts solar into chemical energy is promising in achieving green energy sustainability, but addressing low electron–hole separation efficiency and sluggish surface kinetic process remains formidable challenges. Herein, a novel CoP@Ni‐CdS Schottky junction composed of Ni‐doped CdS nanorods and quasi‐metallic CoP nanoparticles is constructed via a simple hydrothermal–calcination method. Experiments and theoretical calculations demonstrate that magnetic Ni‐doping not only induces a spin‐polarized electric field and enhances the built‐in interfacial electric field strength, but also rises the Schottky barrier height at the heterointerface, which synergistically accelerates the separation efficiency of photoinduced charges and modulates the electronic configuration of the active site to optimize the adsorption–desorption behaviors for H2O molecules and H* intermediates. Therefore, the designed CoP@Ni‐CdS catalyst exhibits an exceptional photocatalytic performance with H2 evolution rate of 42.14 mmol g−1 h−1 with the apparent quantum efficiencies of 16.8% at 420 nm, which is 14.14 and 2.21 times higher than that of pristine CdS and Ni‐CdS, respectively. This work provides in‐depth insights into fabricating dual electric fields, tuning the Schottky barrier and modulating the electronic configuration of active sites in Schottky heterojunction for ameliorative photocatalytic activity.

Efficient photocatalytic degradation of methylene blue via synergistic dual co-catalyst on SrTiO3@Al under visible light: Experimental and DFT study

BackgroundPhotocatalytic oxidation is a green method for water purification. However, the operation of traditional photocatalysts depends on exposure to UV radiation, which only forms a small portion of the spectrum comprising sunlight. The expansion of photocatalyst absorption to the visible range of light could greatly improve the efficiency and economic viability of the process. MethodsThe photocatalyst was prepared by first synthesising SrTiO3 nanoparticles by chemical precipitation followed by calcination. Then, SrTiO3 was doped with aluminium using a flux method with Al2O3 and SrCl2 at 1150 °C. Finally, the dual co-catalysts, Rh/Cr2O3 and CoOOH, were photodeposited onto SrTiO3@Al via sequential irradiation. Significant findingsThe Rh/Cr2O3/SrTiO3@Al/CoOOH nanocomposite degraded 87% of methylene blue (MB) (10 mg/L) under visible light in 1 h, a 3.3-fold improvement over pure SrTiO3 and 2.1-fold over a similar commercial composite. This enhancement is due to efficient charge separation resulting from Al doping and improved carrier transport as a result of the anisotropic deposition of the co-catalysts. Optimisation showed that 20 mg of photocatalyst in 50 mL of MB solution (5 mg/L) degraded 100% thereof within 45 min. DFT calculations showed uneven electron distribution in SrTiO3′s conduction band and structural changes with Al doping, further enhancing photocatalytic activity.

Introducing Oxygen Vacancies into a WO3 Photoanode through NaH2PO2 Treatment for Efficient Water Splitting.

WO3, with a high light absorption capacity and a suitable band structure, is considered a promising photoanode material for photoelectrochemical water splitting. However, the poor photoinduced electron-hole separation efficiency limits its application. Herein, we report an effective strategy to suppress electron-hole recombination by introducing oxygen vacancies (OV) on the surface of a WO3 photoanode through NaH2PO2 treatment. An OV-enriched amorphous surface layer with a thickness of 4 nm is formed after NaH2PO2 treatment, which increases the charge carrier density and enlarges the electrochemical surface area of the photoanode. The charge separation and surface injection efficiencies are both improved after NaH2PO2 treatment, and the charge transfer process of the photoanode is accelerated consequently. The current density of the modified WO3 photoanode reaches 0.96 mA cm-2 at 1.23 V.

Enhanced Photodegradation of Congo Red Using RSM‐Optimized TiO₂ on Borassus flabellifer Male Inflorescence Biochar

AbstractThis study explores the use of biochar, derived from Borassus flabellifer male inflorescence biomass as an alternative support for titanium dioxide (TiO2) to enhance its photocatalytic activity in degrading Congo red (CR) dye pollutant. The biochar was synthesized through controlled pyrolysis and subsequently combined with TiO2 to form a nanocomposite via hydrothermal method. The primary goal of creating this nanocomposite is to breakdown azo dyes, such as CR, using UV irradiation. Comprehensive characterization techniques, including XRD, FTIR, SEM coupled with EDAX, XPS, and UV‐DRS confirmed the successful integration of biochar with TiO2. The enhanced photocatalyst performance is attributed to the increased surface area, improved light absorption, and efficient charge separation facilitated by the biochar support. Furthermore, the experimental parameters were optimized using the response surface methodology (RSM). These studies demonstrated that the CR concentration, contact duration, pH, and photocatalyst quantity are critical factors in the photocatalytic oxidation process. The strong correlation coefficient for the first order model indicated that the data described by the RSM, agreed with the obtained results. This study highlights the potential of agricultural waste‐derived biochar as a cost‐effective and sustainable support for TiO₂, offering a viable solution for the remediation of dye‐contaminated water.

The Role of Thermally Activated Charge Separation in Organic Solar Cells

AbstractIn recent years, organic solar cells (OSCs) have shown high power efficiencies approaching 20%. However, the fundamental mechanisms of charge separation in these highly efficient devices have been a subject of intensive debates. Here, the charge separation efficiency (CSE) is extensively investigated across a wide range of blend systems with different energetic offsets. The findings unveil the temperature‐dependent nature of charge separation in low‐offset systems, emphasizing its significant contribution to the overall CSE. An intriguing inverse correlation between CSE and charge separation activation energy in relation to the offset is also observed. These results shed new light on the factors underlying the high CSE observed in the state‐of‐the‐art devices.

Photoelectrodes with Enhanced Carrier Generation and Collection Through Optical Simulation and Materials Engineering

AbstractThe efficiency of solar‐fuel conversion in photoelectrochemical (PEC) systems is hindered by significant losses of photons and photocarriers within the photoelectrodes. This study introduces an innovative ITO@In2S3 core‐shell nanowire structure designed to overcome these challenges through cutting‐edge materials engineering and sophisticated simulation techniques. Optical modeling and finite element simulations highlight the conflict between photocarrier generation and collection in planar In2S3 thin films and demonstrate how the core‐shell nanowire geometry can significantly enhance light absorption. The developed ITO@In2S3 nanowire photoanodes achieve a photocurrent of 11.3 mA cm−2 at 1.23 V versus RHE, which is nearly five times greater than that of planar ITO/In2S3 thin films. Characterization techniques, including UV–vis absorption and charge separation efficiency measurements, confirm the enhanced light absorption and improved carrier collection facilitated by broadening the optical absorption range and reducing carrier transport distances. This research not only deepens the understanding of the dynamics within thin‐film photoelectrodes but also paves the way for the development of more efficient technologies for solar fuel conversion.

Dipole polarization modulating of vinylene-linked covalent organic frameworks for efficient photocatalytic hydrogen evolution

Photocatalytic hydrogen (H2) evolution using covalent organic frameworks (COFs) is an attractive and promising avenue for exploration, but one of its big challenges is low photo-induced charge separation. In this study, we present a straightforward and facile dipole polarization engineering strategy to enhance charge separation efficiency, achieved through atomic modulation (O, S, and Se) of the COF monomer. Our findings demonstrate that incorporating atoms with varying electronegativities into the COF matrix significantly influences the local dipole moment, thereby affecting charge separation efficiency and photostability, which in turn affects the rates of photocatalytic H2 evolution. As a result, the newly developed TMT-BO-COF, which contains highly electronegative O atoms, exhibits the lowest exciton binding energy, the highest efficiency in charge separation and transportation, and the longest lifetime of the active charges. This leads to an impressive average H2 production rate of 23.7 mmol g−1 h−1, which is 2.5 and 24.5 times higher than that of TMT-BS-COF (containing S atoms) and TMT-BSe-COF (containing Se atoms), respectively. A novel photocatalytic hydrogen evolution mechanism based on proton-coupled electron transfer on N in the structure of triazine rings in vinylene-linked COFs is proposed by theoretical calculations. Our findings provide new insights into the design of highly photoactive organic framework materials for H2 evolution and beyond.

Unraveling the roles of atomically-dispersed Au in boosting photocatalytic CO2 reduction and aryl alcohol oxidation

Atomically-dispersed metal-based materials represent an emerging class of photocatalysts attributed to their high catalytic activity, abundant surface active sites, and efficient charge separation. Nevertheless, the roles of different forms of atomically-dispersed metals (i.e., single-atoms and atomic clusters) in photocatalytic reactions remain ambiguous. Herein, we developed an ethylenediamine (EDA)-assisted reduction method to controllably synthesize atomically dispersed Au in the forms of Au single atoms (AuSA), Au clusters (AuC), and a mixed-phase of AuSA and AuC (AuSA+C) on CdS. In addition, we elucidate the synergistic effect of AuSA and AuC in enhancing the photocatalytic performance of CdS substrates for simultaneous CO2 reduction and aryl alcohol oxidation. Specifically, AuSA can effectively lower the energy barrier for the CO2→*COOH conversion, while AuC can enhance the adsorption of alcohols and reduce the energy barrier for dehydrogenation. As a result, the AuSA and AuC co-loaded CdS show impressive overall photocatalytic CO2 conversion performance, achieving remarkable CO and BAD production rates of 4.43 and 4.71 mmol g−1 h−1, with the selectivities of 93% and 99%, respectively. More importantly, the solar-to-chemical conversion efficiency of AuSA+C/CdS reaches 0.57%, which is over fivefold higher than the typical solar-to-biomass conversion efficiency found in nature (ca. 0.1%). This study comprehensively describes the roles of different forms of atomically-dispersed metals and their synergistic effects in photocatalytic reactions, which is anticipated to pave a new avenue in energy and environmental applications.